Given the abundant solar light available on our planet, it is promising to develop an advanced fabric capable of simultaneously providing personal thermal management and facilitating clean water production in an energy-efficient manner. In this study, we present the fabrication of a photothermally active, biodegradable composite cloth composed of titanium carbide MXene and cellulose, achieved through an electrospinning method. This composite cloth exhibits favorable attributes, including chemical stability, mechanical performance, structural flexibility, and wettability. Notably, our 0.1-mm-thick composite cloth (RC/MXene IV) raises the temperature of simulated skin by 5.6 degrees C when compared to a commercially available cotton cloth, which is five times thicker under identical ambient conditions. Remarkably, the composite cloth (RC/MXene V) demonstrates heightened solar light capture efficiency (87.7%) when in a wet state instead of a dry state. Consequently, this cloth functions exceptionally well as a high-performance steam generator, boasting a superior water evaporation rate of 1.34 kg m(-2) h(-1) under one-sun irradiation (equivalent to 1000 W m(-2)). Moreover, it maintains its performance excellence in solar desalination processes. The multifunctionality of these cloths opens doors to a diverse array of outdoor applications, including solar-driven water evaporation and personal heating, thereby enriching the scope of integrated functionalities for textiles.
Maintaining human thermal comfort in the cold outdoors is crucial for diverse outdoor activities, e.g., sports and recreation, healthcare, and special occupations. To date, advanced clothes are employed to collect solar energy as a heat source to stand cold climates, while their dull dark photothermal coating may hinder pragmatism in outdoor environments and visual sense considering fashion. Herein, tailor-made white webs with strong photothermal effect are proposed. With the embedding of cesium–tungsten bronze (CsxWO3) nanoparticles (NPs) as additive inside nylon nanofibers, these webs are capable of drawing both near-infrared (NIR) and ultraviolet (UV) light in sunlight for heating. Their exceptional photothermal conversion capability enables 2.5–10.5 °C greater warmth than that of a commercial sweatshirt of six times greater thickness under different climates. Remarkably, this smart fabric can increase its photothermal conversion efficiency in a wet state. It is optimal for fast sweat or water evaporation at human comfort temperature (38.5 °C) under sunlight, and its role in thermoregulation is equally important to avoid excess heat loss in wilderness survival. Obviously, this smart web with considerable merits of shape retention, softness, safety, breathability, washability, and on-demand coloration provides a revolutionary solution to realize energy-saving outdoor thermoregulation and simultaneously satisfy the needs of fashion and aesthetics.
Graphene oxide (GO) is a classic two dimensional (2D) building block that can be used to develop high-performance materials for numerous applications, particularly in the energy and environmental fields. Currently, the precise assembly of GO nanosheets into macroscopic nanohybrids of superior strength and toughness is desirable, and faces challenges and trade-offs. Herein, we exploited the freshly established polycationitrile method as a powerful molecular crosslinking strategy to engineer ultratough and ultrastrong GO/polymer hybrid films, in which a covalent triazine-based network was constructed in a mild condition to reinforce the interface between GO nanosheets. The tensile strength and toughness reached 585 +/- 25 MPa and 14.93 +/- 1.09 MJ m(-3), respectively, which, to the best of our knowledge, are the current world records in all GO-based hybrid films. As an added merit of the tailor-made polymer crosslinker, the high mechanical performance can be maintained in large part at an extremely high relative humidity of 98%. This emerging interface-engineering approach paves a new avenue to produce integrated strong-and-tough 2D nanohybrid materials that are useful in aerospace, artificial muscle, energy harvesting, tissue engineering and more.
Graphene and its derivatives are a classical group of two-dimensional (2D) building blocks possessing excellent mechanical and/or electrical properties in favor of preparing flexible electronic devices. Natural materials, such as nacre, provide inspiration and an exciting guideline for assembling 2D nanosheets into functional nanocomposites. In this context, despite recent advance, methods to assemble graphene-derived nanosheets into nanocomposites with the integrated enhancement of mechanical properties and electrical conductivity are eagerly pursued. Here, a rational design has been proposed and demonstrated, which utilizes synergistic supramolecular interactions between a polymeric additive and reduced graphene-oxide nanosheets to fabricate exceptional, integrated, strong, and tough nanocomposite films with high electrical conductivity. Such materials can be applied in areas such as, aerospace, artificial muscle, tissue engineering, and flexible electronics.
Noble metals are the most commonly used electrocatalysts, but due to the high-cost and scarcity, improving their utilization has become a hot topic. As the Pt-based high-entropy alloy (HEA) can greatly increase the activity of catalyst and increase the utilization of noble metal, herein, a HEA with promising performance in ethylene glycol oxidation reaction (EGOR) is developed. The EGOR results show that, the onset potential of PtPdAuNiCo/C is 0.55 V, which is 20 mV lower than Pt/C (0.57 V) reference. Besides, the PtPdAuNiCo/C exhibits a high activity of 0.482 A mg−1PtPdAu, which is 2.18 times of Pt/C (0.221 A mg−1Pt) reference. And the current retention rate of PtPdAuNiCo/C (81.3%) is also higher than Pt/C (73.0%) reference in 500-cycle stability test. When as-obtained PtPdAuNiCo/C assembled into a direct ethylene glycol fuel cell, it exhibits a high-power density of 8.38 mW cm−2. It is 1.40 times than that of Pt/C (6.00 mW cm−2) reference. This work would be a good reference to HEA materials application on electrocatalysis in future.
Inhomogeneous lithium-ion (Li+) deposition is one of the most crucial problems, which severely deteriorates the performance of solid-state lithium metal batteries (LMBs). Herein, we discovered that covalent organic framework (COF-1) with periodically arranged boron-oxygen dipole lithiophilic sites could directionally guide Li+ even deposition in asymmetric solid polymer electrolytes. This in situ prepared 3D cross-linked network Poly(ACMO-MBA) hybrid electrolyte simultaneously delivers outstanding ionic conductivity (1.02 × 10−3 S cm−1 at 30 °C) and excellent mechanical property (3.5 MPa). The defined nanosized channel in COF-1 selectively conducts Li+ increasing Li+ transference number to 0.67. Besides, The COF-1 layer and Poly(ACMO-MBA) also participate in forming a boron-rich and nitrogen-rich solid electrolyte interface to further improve the interfacial stability. The Li‖Li symmetric cell exhibits remarkable cyclic stability over 1000 h. The Li‖NCM523 full cell also delivers an outstanding lifespan over 400 cycles. Moreover, the Li‖LiFePO4 full cell stably cycles with a capacity retention of 85% after 500 cycles. the Li‖LiFePO4 pouch full exhibits excellent safety performance under pierced and cut conditions. This work thereby further broadens and complements the application of COF materials in polymer electrolyte for dendrite-free and high-energy-density solid-state LMBs.
Developing inexpensive but efficient electrocatalysts for oxygen reduction reactions (ORR) is critical to the design of zinc-air battery (ZAB). Here, we report a good ORR electrocatalyst (MoFeCx-NC) composed of nitrogen-doped carbon armored by ferro-molybdenum binary carbides. The physical characterization of MoFeCx-NC by X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) show that MoFeCx-NC is composed of amorphous bimetallic carbides and N-doped carbon. In addition, the electrochemical test shows that its more positive onset potential of 0.962 V and better half-wave potential of 0.847 V, almost close to Pt/C (Eonset = 0.957 V, E1/2 = 0.854 V). Furthermore, the MoFeCx-NC assembled ZAB exhibits a good peak power density of 79.14 mW cm−2 and an impressive 1.40 V discharge voltage, indicating that the obtained MoFeCx-NC is an ideal for the future ORR electrocatalyst.
Diphenolic acid (DPA) is a kind of endocrine-disrupting compound, which brings serious health problems to humans and animals. An eco-friendly and cost-effective adsorbent was prepared through a simple method, in which the β-Cyclodextrin(β-CD) was crosslinked onto the surface of diatomite (DA), the as-prepared DA/β-CD composite showed higher adsorption efficiency for DPA than DA as the host–guest interaction between DPA and β-CD. DA is a kind of biosilica with a hierarchical pore structure that provides enough surface area for the DA/β-CD. The surface area and pore size of DA/β-CD were investigated by nitrogen adsorption and desorption. The DA/β-CD composite illustrated a good adsorption capability, and was used for removing DPA from wastewater. The adsorption ratio of DPA could achieve 38% with an adsorption amount of 9.6 mg g−1 under room temperature at pH = 6. The adsorption isotherm curves followed the Langmuir (R2 = 0.9867) and Freundlich (R2 = 0.9748) models. In addition, the regeneration rate of the DA/β-CD was nearly at 80.32% after three cycles of regeneration. These results indicated that the DA/β-CD has the potential for practical removal of the EDC contaminants from wastewater.
Bilayer actuators, traditionally consisting of two laminated materials, are the most common types of soft or hybrid actuators. Herein, a nanomaterial-based organic–inorganic humidity-sensitive bilayer actuator composed of TEMPO-oxidized cellulose nanofibrils (TCNF-Na+) and reduced graphene oxide (rGO) sheets is presented. The hybrid actuator displays a large humidity-driven locomotion with an atypical fast unbending. Cationic exchange of the anionically charged TCNF-Na+ and control of the layer thickness is used to tune and dictate the locomotion and actuator's response to humidity variations. Assembly of a self-oscillating electrical circuit, that includes a conductive rGO layer, displays autonomous on-and-off lighting in response to actuation-driven alternating electrical heating.
Herein, we established a synthetic route towards MXene/poly(ionic liquid) (PIL) composite porous membranes as a new platform of solar-thermal conversion materials. These membranes were made by a base-triggered ionic crosslinking process between a cationic PIL and a weak polyacid in solution in the presence of dispersed MXene nanosheets. A three-dimensionally interconnected porous architecture was formed with MXene nanosheets uniformly distributed within it. The unique characteristics of the as-produced composite membranes displays significant light-to-heat conversion and excellent performance for solar-driven water vapor generation. This facile synthetic strategy opens a new avenue for developing composite porous membranes as solar absorbers for the solar-driven water production from natural resources.
Controlled synthesis of polymer-based porous membranes via innovative methods is of considerable interest, yet it remains a challenge. Herein, we established a general approach to fabricate porous polyelectrolyte composite membranes (PPCMs) from poly-(ionic liquid) (PIL) and MXene via an ice-assisted method. This process enabled the formation of a uniformly distributed macroporous structure within the membrane. The unique characteristics of the as-produced composite membranes display significant light-to-heat conversion and excellent performance for solar-driven water vapor generation. This facile synthetic strategy breaks new ground for developing composite porous membranes as high-performance solar steam generators for clean water production.
Controlled regulation of polymer-based porous membranes via innovative methods is of considerable interest yet it remains a challenge. Herein, we established a general approach to fabricate porous polyelectrolyte composite membranes (PPCM)s from poly(ionic liquid) (PIL) and MXene via an ice-templating method. This process enabled the formation of a uniformly distributed macroporous structure within the membrane. The unique characteristics of the as-produced composite membranes displays significant light-to-heat conversion and excellent performance for solar-driven water vapor generation. This facile synthetic strategy breaks new grounds for developing composite porous membranes as high-performance solar steam generator for clean water production.
Carbon nanotubes (CNTs) have received considerable attention for their excellent thermal and electrical conductivity as well as scalable production. However, CNT dispersions are prone to settling and have a short shelf time, especially under high concentration, which significantly hinders their further processing and increases transportation costs. Here, we report a highly concentrated CNT dough enabled by ionic liquid crystal (ILC) as auxiliaries. Benefiting from the temperature-controlled physical transformation of the ILC, the CNTs of the powder state are successfully transferred to highly processable dough with excellent electrical conductivity, flame retardancy, and outstanding redispersibility even after 180 days of storage. In particular, the CNT dough exhibits excellent self-healing properties and good reshapable capability. Various bulk form CNT derived from the ILC armored CNT dough are realized by facile processing technique. Hybrid nanocomposite papers with ANF nanofiber exhibited excellent photothermal conversion and Joule heating properties. The redispersible CNT doughs presented here promise to revolutionize traditional CNT powder and dispersions as the primary raw material for building CNT-based architectures and facilitate the large-scale application of CNTs.
Assembling two-dimensional (2D) materials by polyelectrolyte often suffers from inhomogeneous microstructures due to the conventional mixing-and-simultaneous-complexation procedure (mix-and-complex) in aqueous solution. Herein a mix-then-on-demand-complex concept via on-demand in situ cascade anionization and ionic complexation of 2D materials is raised that drastically improves structural order in 2D assemblies, as exemplified by classical graphene oxide (GO)-based ultrathin membranes. Specifically, in dimethyl sulfoxide, the carboxylic acid-functionalized GO sheets (COOH-GOs) were mixed evenly with a cationic poly(ionic liquid) (PIL) and upon filtration formed a well-ordered layered composite membrane with homogeneous distribution of PIL chains in it; next, whenever needed, it was alkali-treated to convert COOH-GO in situ into its anionized state COO--GO that immediately complexed ionically with the surrounding cationic PIL chains. This mix-then-on-demand-complex concept separates the ionic complexation of GO and polyelectrolytes from their mixing step. By synergistically combining the PIL-induced hydrophobic confinement effect and supramolecular interactions, the as-fabricated nanofiltration membranes carry interface transport nanochannels between GO and PIL, reaching a high water permeability of 96.38 L m(-2) h(-1) bar(-1) at a maintained excellent dye rejection 99.79% for 150 h, exceeding the state-of-the-art GO-based hybrid membranes. The molecular dynamics simulations support the experimental data, confirming the interface spacing between GO and PIL as the water transport channels.
Two-dimensional (2D) MXene-based lamellar membranes play transformative roles in membrane filtration technology. Their practical use in water treatment is however hindered by several hurdles, e.g., unfavorable swelling due to weak interactions between adjacent MXene nanosheets, tortuous diffusion pathways of layered stacking, and the intrinsic aquatic oxidation-prone nature of MXene. Herein, nanoporous 2D/2D heterostructure membranes are elaborately constructed via solution-phase assembly of oppositely charged MXene and modified layered double hydroxide (MLDH) nanosheets. As a multifunctional component, positively charged holey MLDH nanosheets were first tailor-made to serve simultaneously as a binder, spacer and surface-modifier; next they were intercalated into negatively charged MXene lamella to enhance structural stability and mass transfer of membranes. As a result, the as-prepared MLDH@MXene heterostructure membranes successfully break the persistent trade-off between high permeability and selectivity while mitigating the common drawbacks in 2D MXene-based lamellar membranes, e.g., swelling issues, restacking problems, and vulnerable chemical stability. Noticeably, at an operating pressure of 4 bar and a feed solution of 100 ppm of Congo red, the heterostructure membranes enable a threefold jump in permeability (332.7 +/- 20 L m(-2) h(-1 )bar(-1)) when compared to the pristine MXene membrane (119.3 +/- 18 L m(-2 )h(-1) bar(-1)), and better operational stability without compromising the rejection.
Two-dimensional (2D) membrane-based ion separation technology has been increasingly explored to address the problem of lithium resource shortage, yet it remains a sound challenge to design 2D membranes of high selectivity and permeability for ion separation applications. Zeolitic imidazolate framework functionalized modified layered double hydroxide (ZIF-8@MLDH) composite membranes with high lithium-ion (Li+) permeability and excellent operational stability were obtained in this work by in situ depositing functional ZIF-8 nanoparticles into the nanopores acting as framework defects in MLDH membranes. The defect-rich framework amplified the permeability of Li+, and the site-selective growth of ZIF-8 in the framework defects bettered its selectivity. Specifically speaking, the ZIF-8@MLDH membranes featured a high permeation rate of Li+ up to 1.73 mol m−2 h−1 and a desirable selectivity of Li+/Mg2+ up to 31.9. Simulations supported that the simultaneously enhanced selectivity and permeability of Li+ are attributed to changes in the type of mass transfer channels and the difference in the dehydration capacity of hydrated metal cations when they pass through nanochannels of ZIF-8. This study will inspire the ongoing research of high-performance 2D membranes through the engineering of defects.
Understanding the reconstruction of surface sites is crucial for gaining insights into the true active sites and catalytic mechanisms. While extensive research has been conducted on reconstruction behaviors of atomically dispersed metallic catalytic sites, limited attention has been paid to non-metallic ones despite their potential catalytic activity comparable or even superior to their noble-metal counterpart. Herein, we report a carbonaceous, atomically dispersed non-metallic selenium catalyst that displayed exceptional catalytic activity in the hydrazine oxidation reaction (HzOR) in alkaline media, outperforming the noble-metal Pt catalysts. In situ X-ray absorption spectroscopy (XAS) and Fourier transform infrared spectroscopy revealed that the pristine SeC4 site pre-adsorbs an ∗OH ligand, followed by HzOR occurring on the other side of the OH–SeC4. Theoretical calculations proposed that the pre-adsorbed ∗OH group pulls electrons from the Se site, resulting in a more positively charged Se and a higher polarity of Se–C bonds, thereby enhancing surface reactivity toward HzO/R.
Fe3C nanoparticles hold promise as catalysts and nanozymes, but their low activity and complex preparation have hindered their use. Herein, this study presents a synthetic alternative toward efficient, durable, and recyclable, Fe3C-nanoparticle-encapsulated nitrogen-doped hierarchically porous carbon membranes (Fe3C/N–C). By employing a simple one-step synthetic method, we utilized wood as a renewable and environmentally friendly carbon precursor, coupled with poly(ionic liquids) as a nitrogen and iron source. This innovative strategy offers sustainable, high-performance catalysts with improved stability and reusability. The Fe3C/N–C exhibits an outstanding peroxidase-like catalytic activity toward the oxidation of 3,3′,5,5′-tetramethylbenzidine in the presence of hydrogen peroxide, which stems from well-dispersed, small Fe3C nanoparticles jointly with the structurally unique micro-/macroporous N–C membrane. Owing to the remarkable catalytic activity for mimicking peroxidase, an efficient and sensitive colorimetric method for detecting ascorbic acid over a broad concentration range with a low limit of detection (~2.64 µM), as well as superior selectivity, and anti-interference capability has been developed. This study offers a widely adaptable and sustainable way to synthesize an Fe3C/N–C membrane as an easy-to-handle, convenient, and recoverable biomimetic enzyme with excellent catalytic performance, providing a convenient and sensitive colorimetric technique for potential applications in medicine, biosensing, and environmental fields.
The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode’s charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g–1 at 10 mV s–1 and superb capacitance retention of 79% at 5000 mV s–1, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm–2, it maintains an impressive capacitance retention of 52% at 1000 mV s–1. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.
In electrocatalytic CO2 reduction reaction (CO2RR), metal-free Se-based multi-doping carbon has become a new focus. In this paper, a series of metal-free Se, B, P, N doped carbon-based catalysts (Se-BP-N-C) were prepared by a simple and scalable pyrolysis method. The electrocatalytic CO2 reduction results show that, the main product on Se-BP-N-C catalyst is CO, and there are no other by-products except H2. Specifically, the optimal one prepared at 1050 °C (named Se-BP-N-C (1050)), can selectively reduce CO2 into CO with Faradaic efficiency (FE) up to 96.2% (at − 0.5 V), and maintains long-term stability after continuous electrolysis for 10 h in a flow cell (current density remained 82.7%). This study would provide a good reference for designing advanced efficient metal-free catalysts in electrocatalysis.
The colloidal polystyrene (PS) was synthesized and decorated with silver nanoparticles (Ag NPs). The plasmonic Ag@PS nanocomposite was prepared by loading Ag NPs on PS microsphere through a seed-mediated in situ growth route. The property of Ag NPs deposited on the PS microsphere could be precisely controlled by adjusting the concentration of the chemicals used in the growth medium. The growth step is only limited by the diffusion of growing species in the growth media to the surface of the Ag seed. The Ag@PS prepared via the in situ growth method exhibited two advantages compared with the self-assembled PS/Ag. First, the high-density of Ag NPs were successfully deposited on the surface of PS as the electroless-deposited Ag seed process, which brings nearly three times SERS enhancement. Second, the rapid preparation process for in situ growth method (half an hour, 10 h for the self-assembled method). The PS/Ag could detect Nile blue A (NBA) down to 10(-7) M by SERS. Furthermore, the plasmonic Ag@PS SERS substrate was used for pesticide identification. The on-site monitoring malachite green (MG) from fish was achieved by portable Raman spectrometer, and the limit of detection (LOD) was 0.02 ppm. The Ag@PS substrate has also shown capability for simultaneously sensing multiple pesticides by SERS.
Heteroatom-doped porous carbon materials (HPCMs) have found extensive applications in adsorption/separation, organic catalysis, sensing, and energy conversion/storage. The judicious choice of carbon precursors is crucial for the manufacture of HPCMs with specific usages and maximization of their functions. In this regard, polymers as precursors have demonstrated great promise because of their versatile molecular and nanoscale structures, modulatable chemical composition, and rich processing techniques to generate textures that, in combination with proper solid-state chemistry, can be maintained throughout carbonization. This Review comprehensively surveys the progress in polymer-derived functional HPCMs in terms of how to produce and control their porosities, heteroatom doping effects, and morphologies and their related use. First, we summarize and discuss synthetic approaches, including hard and soft templating methods as well as direct synthesis strategies employing polymers to control the pores and/or heteroatoms in HPCMs. Second, we summarize the heteroatom doping effects on the thermal stability, electronic and optical properties, and surface chemistry of HPCMs. Specifically, the heteroatom doping effect, which involves both single-type heteroatom doping and codoping of two or more types of heteroatoms into the carbon network, is discussed. Considering the significance of the morphologies of HPCMs in their application spectrum, potential choices of suitable polymeric precursors and strategies to precisely regulate the morphologies of HPCMs are presented. Finally, we provide our perspective on how to predefine the structures of HPCMs by using polymers to realize their potential applications in the current fields of energy generation/conversion and environmental remediation. We believe that these analyses and deductions are valuable for a systematic understanding of polymer-derived carbon materials and will serve as a source of inspiration for the design of future HPCMs.
Recently, nitrogen-doped porous carbon materials containing non-precious metals (termed “M-N-C”) have formed a group of functional materials to replace precious metal-based catalysts for electrochemical CO2 reduction reaction. Here, a series of mesoporous Ni-N-C electrocatalysts (termed “mp-Ni-N-Cs”) were prepared via a gel-template method, and could effectively reduce CO2 into CO in a flow cell. The result in gas sorption tests exhibited a typical mesoporous structure, which would bring both sufficient exposed active sites and convenient mass transfer channels. Electrochemical tests showed excellent performance at an applied potential of -1.3 V (vs. RHE), e.g., a CO Faradaic efficiency (FECO) of 95.85 %, and a CO reduction current (jCO) of -21.29 mA cm−2. Significantly, its FECO exceeded 93 % in a wide range of potentials from -1.0 to -1.5 V, showing great tolerance to fluctuation in potential. The mp-Ni-N-C electrocatalysts have satisfactory features in terms of catalytic activity, facile preparation, and economic feasibility, and will offer a valuable reference for next exploration of cost-effective electrocatalysts for CO2 conversion.
Cost-effective heteroatom-doped porous carbons are considered promising electrocatalysts for CO2 reduction reaction (CO2RR). Traditionally porous carbons with N doping or N/X codoping (X denotes the second type of heteroatom) have been widely studied, leaving ternary doping a much less studied yet exciting topic to be explored. Herein, a series of electrocatalysts based on metal-free Se, B, and N ternary-doped porous carbons (termed “SeBN-Cs”) were synthesized and tested as metal-free electrocatalysts in CO2RR. Our study indicates that the major product of CO2RR on the SeBN-C electrocatalysts was CO with a small fraction (<5%) of H2 as the byproduct. The optimal electrocatalyst sample SeBN-C-1100 prepared at 1100 °C exhibits a high CO selectivity with a Faradaic efficiency of CO reaching 95.2%. After 10 h of continuous electrolysis operation, the Faradaic efficiency and the current density are maintained high at 97.6 and 84.7% of the initial values, respectively, indicative of a long-term operational stability. This study provides an excellent reference to deepen our understanding of the properties and functions of multi-heteroatom-doped porous carbon electrocatalysts in CO2RR.
Background: As a promising green energy conversion device, direct ethylene glycol fuel cells (DEGFC) have been widely studied. But high-cost of their catalysts has severely limited large-scale commercial application. Developing economic and effective anodic electrocatalyst is an urgent work presently.
Methods: Herein, an efficient high entropy alloy catalyst (HEA, penta-element) was prepared. Then, their catalytic performance and properties were authenticated by some electrochemical and physical methods. Importantly, it was also applied to a real DEGFC stack.
Significant findings: Notably, the ethylene glycol oxidation current density (0.65 A mg−1PtPdAu) on as-prepared HEA is three times than that of commercial Pt/C (0.22 A mg−1Pt) with good long-term durability. Moreover, the HEA-equipped DEGFC obtains an open circuit potential of 0.58 V, which delivers 2 times larger peak power density (17.63 mW cm−2) than that of commercial Pt/C (7.37 mW cm−2). This work would be a good reference to developing other advanced HEA materials in electrocatalytic fields.
The rational design of catalytically active sites in porous materials is essential in electrocatalysis. Herein, atomically dispersed Fe-N-x sites supported by hierarchically porous carbon membranes are designed to electrocatalyze the hydrazine oxidation reaction (HzOR), one of the key techniques in electrochemical nitrogen transformation. The high intrinsic catalytic activity of the Fe-N-x single-atom catalyst together with the uniquely mixed micro-/macroporous membrane support positions such an electrode among the best-known heteroatom-based carbon anodes for hydrazine fuel cells. Combined with advanced characterization techniques, electrochemical probe experiments, and density functional theory calculation, the pyrrole-type Fe-N-4 structure is identified as the real catalytic site in HzOR.
Solar powered clean water production has been considered a favorable way to address the problem of the global water shortage. Recently, the interfacial solar-steam generation system has greatly improved water evaporation by localizing the solar energy at an advanced solar-thermal conversion material interface. However, the specific water productivity (SWP) is still far away from a satisfactory level due to the strong mutual interference between the incident sunlight and the generated water vapor, which causes a huge loss in energy and in turn restrains the final efficiency in water evaporation and collection. SWP is the water collection per solar radiation area per hour, which reflects the actual solar efficiency for water production and a key concern in desalination. Herein, we report a rational Janus-interface solar-steam generator (J-SSG), which separates the water evaporation and the solar-thermal conversion on the two sides of the film generator. This J-SSG demonstrates a water evaporation rate of up to 2.21 kg m(-2) h(-1) under 1 sun in a large area of 100 cm(2). More importantly, a record high SWP of 1.95 kg m(-2) h(-1) is realized in a simple system, and the SWP efficiency corresponding to the ratio of SWP to evaporation rate is as high as 88%. In an outdoor test (Beijing, solar energy similar to 15 MJ m(-2) day(-1)), 10 L purified water per square meter have been easily achieved. This Janus-interface engineering of the solar-steam generator provides a novel strategy and solution for solar powered water production of practical significance.
A series of organic phosphonic acids (OPAs) were applied as multifunctional spacers to enlarge the inner space of carbide MXene (Ti3C2Tx) laminates. A synergistic improvement in permeance, rejection and stability is achieved via introducing OPA to create pillared laminates. This strategy provides a universal way to regulate transport channels of MXene-based membranes.
Two-dimensional (2D) MXene-based lamellar membranes bearing interlayers of tunable hydrophilicity are promising for high-performance water purification. The current challenge lies in how to engineer the pore wall's surface properties in the subnano-confinement environment while ensuring its high selectivity. Herein, poly(ionic liquid)s, equipped with readily exchangeable counter anions, succeeded as a hydrophilicity modifier in addressing this issue. Lamellar membranes bearing nanochannels of tailorable hydrophilicity are constructed via assembly of poly(ionic liquid)-armored MXene nanosheets. By shifting the interlayer galleries from being hydrophilic to more hydrophobic via simple anion exchange, the MXene membrane performs drastically better for both the permeance (by two-fold improvement) and rejection (≈99 %). This facile method opens up a new avenue for building 2D material-based membranes of enhancing molecular transport and sieving effect.
The integration of surface-enhanced Raman scattering (SERS) spectroscopy with magnetic fluid provides significant utility in point-of-care (POC) testing applications. Bifunctional magnetic–plasmonic composites have been widely employed as SERS substrates. In this study, a simple and cost-effective approach was developed to synthesize magnetic–plasmonic SERS substrates by decorating silver nanoparticles onto magnetic Fe3O4 nanoparticles (AgMNPs), which function both as SERS-active substrates and magnetic fluid particles. The strong magnetic responsivity from AgMNPs can isolate, concentrate, and detect target analytes from the irregular surface of fish skin rapidly. We fabricate a microfluid chip with three sample reservoirs that confine AgMNPs into ever smaller volumes under an applied magnetic field, which enhances the SERS signal and improves the detection limit by two orders of magnitude. The magnetic fluid POC sensor successfully detected malachite green from fish with excellent selectivity and high sensitivity down to the picomolar level. This work achieves a label-free, non-destructive optical sensing approach with promising potential for the detection of various harmful ingredients in food or the environment.
High-frequency responsive capacitors with lightweight, flexibility, and miniaturization are among the most vital circuit components because they can be readily incorporated into various portable devices to smooth out the ripples for circuits. Electrode materials no doubt are at the heart of such devices. Despite tremendous efforts and recent advances, the development of flexible and scalable high-frequency responsive capacitor electrodes with superior performance remains a great challenge. Herein, a straightforward and technologically relevant method is reported to manufacture a carbon fabric membrane “glued” by nitrogen-doped nanoporous carbons produced through a polyelectrolyte complexation-induced phase separation strategy. The as-obtained flexible carbon fabric bearing a unique hierarchical porous structure, and high conductivity as well as robust mechanical properties, serves as the free-standing electrode materials of electrochemical capacitors. It delivers an ultrahigh specific areal capacitance of 2632 µF cm−2 at 120 Hz with an excellent alternating current line filtering performance, fairly higher than the state-of-the-art commercial ones. Together, this system offers the potential electrode material to be scaled up for AC line-filtering capacitors at industrial levels.
Ti3C2Tx (MXene), a thriving member of the two-dimensional (2D) materials family, has shown increasing potential in a myriad of applications, ranging from printable electronics to energy storage and separation membranes. Nevertheless, the dilemma of its oxidative instability and the easy disintegration of its assemblies in contact with water has been restricting its real-life use. Here, we report the benefits of tartaric acid, a natural source, as a non-innocent additive in the MXene composite. In water, it can, above all, inhibit oxidation of Ti3C2Tx and hold individual components in the composite Ti3C2Tx/poly(3,4-ethylenedioxy thiophene):polystyrene sulfonate) (Ti3C2Tx/PEDOT:PSS) firmly together; equally important, it can boost 4-fold the composite’s electron conductivity in comparison to the additive-free equivalent. To showcase its practical value, a tartaric-acid-treated, water-stable MXene/PEDOT:PSS conductive coating is made, which serves as electrodes for an ultrafast supercapacitor; among all 2D materials-based assemblies, the designed supercapacitor delivers, to our knowledge, the record-high performance in an alternating-current filtering application.
Ultrafast electrochemical capacitors with alternating current line filtering function have attracted growing attention owing to their potential to replace the state-of-the-art bulky aluminum electrolyte capacitors. In spite of rapid advance recently involving nanomaterials as electrode building units, it remains largely unexplored how to structurally and chemically engineer electrodes out of renewable resource with competitive or better rate performance. Herein, wood as a renewable resource was used to fabricate highly conductive, robust, porous thin carbon membranes as free-standing electrodes for ultrafast electrochemical capacitors. Transformation of wood slice to carbon membrane proceeds via wet-chemical treatment of wood slices and subsequent morphology maintaining carbonization by spark plasma sintering. Judiciously combining high conductivity, characteristic porous architecture with low tortuosity and high continuity, and the ultrathin thickness down to 20 ism, the carbon membrane-based electrochemical capacitor exhibits excellent frequency response with efficient 120 Hz filtering (phase angle = - 83.5 degrees). Compared to the latest electrodes for line filtering application that are fabricated from carbon nanotubes, graphene, and MXene, the wood-derived carbon membranes possess a competitive specific areal capacitance of up to 509.7 mu F cm(-2), and extremely low resistance-capacitance constant of 164.7 mu s, plus the inexpensive scalable fabrication strategy.
Poly(ionic liquid)s (PILs), as an innovative class of polyelectrolytes, are composed of polymeric backbones with IL species in each repeating unit. The combined merits of the polymers and ILs make them promising materials for composites in materials science. Particularly, the integration of PILs with functional substances (PIL composites) opens up a new dimension in utilizing ionic polymers by offering novel properties and improved functions, which impacts multiple subfields of our chemical society. This review summarizes recent developments of PIL composites with a special emphasis on the preparation techniques that are based on the intrinsic properties of the PILs and the synergistic effects between the PILs and substances of interest for diverse applications.
High energy/power density, capacitance, and long-life cycles are urgently demanded for energy storage electrodes. Porous carbons as benchmark commercial electrode materials are underscored by their (electro)chemical stability and wide accessibility, yet are often constrained by moderate performances associated with their powdery status. Here via controlled vacuum pyrolysis of a poly(ionic liquid) membrane template, advantageous features including good conductivity (132 S cm(-1) at 298 K), interconnected hierarchical pores, large specific surface area (1501 m(2) g(-1)), and heteroatom doping are realized in a single carbon membrane electrode. The structure synergy at multiple length scales enables large areal capacitances both for a basic aqueous electrolyte (3.1 F cm(-2)) and for a symmetric all-solid-state supercapacitor (1.0 F cm(-2)), together with superior energy densities (1.72 and 0.14 mW h cm(-2), respectively) without employing a current collector. In addition, theoretical calculations verify a synergistic heteroatom co-doping effect beneficial to the supercapacitive performance. This membrane electrode is scalable and compatible for device fabrication, highlighting the great promise of a poly(ionic liquid) for designing graphitic nanoporous carbon membranes in advanced energy storage.