Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among...Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.展开更多
Oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are the key reactions in numerous renewable energy devices. Unlike conventional powdered catalysts, self-supported catalysts are extensively employed i...Oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are the key reactions in numerous renewable energy devices. Unlike conventional powdered catalysts, self-supported catalysts are extensively employed in oxygen electrocatalysis because of the enhanced electron-transfer rate, high specific surface area, and superior mechanical flexibility. Among the self-supported conductive substrates, carbon fiber usually exhibits several distinctive advantages, such as a straightforward preparation process, relatively low cost, good stability, and excellent conductivity. Against this background,carbon fiber-based self-supported electrocatalysts have been widely applied and studied in oxygen electrocatalysis, indicating a promising development direction in oxygen electrocatalyst research.Thus, it is essential to offer an overall summary of the research progress in this field to facilitate its subsequent development. Taking the regulatory mechanisms and modification methods as a starting point, this review comprehensively summarizes recent research on carbon fiber-based self-supported electrocatalysts in recent years. Firstly, a brief overview of the synthesis methods and regulatory mechanisms of carbon fiber-based self-supported electrocatalysts is given. Furthermore, the view also highlights the modification methods and research progress of self-supported electrocatalysts synthesized on carbon fiber-based substrates in recent years in terms of different dopant atoms. Finally, the prospects for the application of self-supported electrocatalysts based on carbon fiber in oxygen electrocatalysis and the possible future directions of their development are presented. This review summarizes recent developments and applications of self-supported bi-functional electrocatalysts with carbon fiber-based materials as the conducting substrate in oxygen electrocatalysis. It also lays a robust scientific foundation for the subsequent reasonable design of highly effective carbon fiber-based self-supported electrocatalysts.展开更多
To meet the practical demand of wearable/portable electronics, developing high-efficiency and durable multifunctional catalyst and in-situ assembling catalysts into electrodes with flexible features are urgently neede...To meet the practical demand of wearable/portable electronics, developing high-efficiency and durable multifunctional catalyst and in-situ assembling catalysts into electrodes with flexible features are urgently needed but challenging. Herein, we report a simple route to fabricate bendable multifunctional electrodes by in-situ carbonization of metal ion absorbed polyaniline precursor. Alloy nanoparticles encapsulated in graphite layer are uniformly distributed in the N-doping carbon nanorod skeleton. Profiting from the favorable free-standing structure and the cooperative effect of metallic nanoparticles, graphitic layer and N doped-carbon architecture, the trifunctional electrodes exhibit prominent activities and stability toward HER, OER and ORR. Notably, due to the protection of carbon layer, the electrocatalysts show the reversible catalytic HER/OER properties. The overall water splitting device can continuously work for 12 h under frequent exchanges of cathode and anode. Importantly, the bendable metal air batteries fabricated by self-supported electrode not only displays the outstanding battery performance,achieving a decent peak power density(125 mW cm^(-2)) and exhibiting favorable charge-discharge durability of 22 h, but also holds superb flexible stability. Specially, a lightweight self-driven water splitting unit is demonstrated with stable hydrogen production.展开更多
Two-dimensional(2D)soft materials,especially in their self-supported forms,demonstrate attractive properties to realize biomimetic morphing and ultrasensitive sensing.Although extensive efforts on design of self-suppo...Two-dimensional(2D)soft materials,especially in their self-supported forms,demonstrate attractive properties to realize biomimetic morphing and ultrasensitive sensing.Although extensive efforts on design of self-supported functional membranes and integrated systems have been devoted,there still remains an unexplored regime of the combination of mechanical,electrical and surface wetting properties for specific functions.Here,we report a self-supported film featured with elastic,thin,conductive and superhydrophobic characteristics.Through a well-defined surface modification strategy,the surface wettability and mechanical sensing can be effectively balanced.The resulted film can function as a smart umbrella to achieve real-time simulated raining with diverse frequencies and intensity.In addition,the integrated umbrella can even response sensitively to the sunlight and demonstrate a positively correlation of current signals with the intensity of sun illumination.Moreover,the superhydrophobic umbrella can be further employed to realize water rescue,which can take the underwater object onto water surface,load and rapidly transport the considerable weight.More importantly,the whole process of loaded objects and water flow velocity can be precisely detected.The self-supported smart umbrella can effectively monitor the weather and realize a smart water rescue,demonstrating significant potentials in multifunctional sensing and directional actuation in the presence of water.展开更多
Amid the ongoing transition toward renewable fuels,the self-supported layered double hydroxides(LDHs)are envisioned as propitious electrocatalysts for reinvigorating the electrocatalysis realm,thereby facilitating env...Amid the ongoing transition toward renewable fuels,the self-supported layered double hydroxides(LDHs)are envisioned as propitious electrocatalysts for reinvigorating the electrocatalysis realm,thereby facilitating environmental remediation and bolstering sustainable global energy security.Exploiting appealing attributes such as unique lamellar structure,abundant active sites,tunable intercalation spacing and compositional flexibility,LDHs boast remarkable activity,selectivity and stability across diverse energy-related applications.By virtue of addressing the technological and time prominence of excavating their renaissance,this review first encompasses the facile state-of-the-art synthetic approaches alongside intriguing modification strategies,toward deciphering the authentic structure–performance correlations for advancing more robust and precise catalyst design.Aside from this,heterostructure engineering employing diversified ranges of coupling materials is highlighted,to construct ground-breaking binder-free LDHs-based heterostructures endowing with unprecedented activity and stability.Subsequently,the milestone gained from experimental research and theoretical modeling of this frontier in multifarious electrocatalytic applications,including HER,OER,UOR,AOR,seawater splitting and other fundamental conversion reactions is rigorously unveiled.As a final note,a brief conclusion is presented with an outline of future prospects.Essentially,this review aspires to offer enlightenment and incite wise inspiration for the future evolution of innovative and resilient next-generation catalysts.展开更多
Hydrogen economy based on electrochemical water splitting exemplified one of the most promising means for overcoming the rapid consumption of fossil fuels and the serious deterioration of global climate.The developmen...Hydrogen economy based on electrochemical water splitting exemplified one of the most promising means for overcoming the rapid consumption of fossil fuels and the serious deterioration of global climate.The development of earth-abundant,efficient,and durable electrocatalysts for hydrogen evolution reaction(HER)plays a vital role in the commercialization of water electrolysis.Regard,the self-supported electrode with unique nitrogen-doped reduced graphene oxide(N-rGO)nanoflakes and WS_(2) hierarchical nanoflower that were grown directly on carbon cloth(CC)substrate(WS_(2)/N-rGO/CC)was successfully synthesized using a facile dual-step hydrothermal approach.The as-synthesized 50%1T/2H-WS_(2)/N-rGO/CC(WGC),which possessed high metallic 1T phase of 57%not only efficiently exposed more active sites and accelerated mass/charge diffusion,but also endowed excellent structural lustiness,robust stability,and durability at a high current density.As a result,the 50%WGC exhibited lower overpotentials and Tafel slopes of 21.13 mV(29.55 mV∙dec^(-1))and 80.35 mV(137.02 mV∙dec^(-1))as compared to 20%Pt-C/CC,respectively for catalyzing acidic and alkaline hydrogen evolution reactions.Pivotally,the as-synthesized 50%WGC also depicted long-term stability for more than 8 h in the high-current-density regions(100 and 220 mA∙cm^(-2)).In brief,this work reveals a self-supported electrode as an extraordinary alternative to Pt-based catalysts for HER in a wide pH range,while paving a facile strategy to develop advanced electrocatalysts with abundant heterointerfaces for practical applications in energy-saving hydrogen production.展开更多
WS2/carbon nanofibers （WS2/CNFs） are obtained by a simple electrospinning method in which few-/ single-layer WS2 is uniformly embedded in carbon fibers. When used as the active anode material for Li-ion cells, these...WS2/carbon nanofibers （WS2/CNFs） are obtained by a simple electrospinning method in which few-/ single-layer WS2 is uniformly embedded in carbon fibers. When used as the active anode material for Li-ion cells, these nanofibers exhibit a first-cycle discharge/charge capacity of 941/756 mAh/g at 100 mAJg and maintain a capacity of 458 mAh/g after 100 cycles at 1 A/g. The evolution of size and crystallinity of WS2 with heating treatment are system- atically studied, which are found to strongly influence the final electrochemical performance. Interestingly, the WS2 samples of lowest crystallinity show the highest performance among all studied samples, which could result from the large interfacial capacity for Li ions due to their large specific surface area. More interestingly, the inherent flexible attribute of electrospun nanofibers renders them a great potential in the utilization of binder-flee anodes. Similar high discharge/charge capacity of 761/604 mAh/g with a first coulombic efficiency of 79.4 % has been achieved in these binder-flee anodes. Considering the universal of such simple and scalable preparation strategy, it is very likely to extend this method to other similar two-dimensional layered materials besides WS2 and provides a promising candidate elec- trode for developing flexible battery devices.展开更多
Developing high-performance anode materials for potassium-ion batteries is significantly urgent. We here demonstrate Sb_2S_3 nanoparticles(~20 nm) homogeneously dispersed in porous S,N-codoped graphene framework(Sb_2S...Developing high-performance anode materials for potassium-ion batteries is significantly urgent. We here demonstrate Sb_2S_3 nanoparticles(~20 nm) homogeneously dispersed in porous S,N-codoped graphene framework(Sb_2S_3-SNG) as a self-supported anode material for potassium-ion batteries. The rational structure design of integrating Sb_2S_3 nanoparticles with S,N-codoped graphene contributes to high reactivity, strong affinity, good electric conductivity, and robust stability of the composite, enabling superior K-storage performance. Moreover, the self-supported architecture significantly decreases the inactive weight of the battery, resulting in a high energy density of a Sb_2S_3-SNG/KVPO_4 F-C full cell to ~166.3 W h kg^(-1).展开更多
Electrolytic water splitting has been considered as a promising technology to produce highly pure H2 by using electrical power produced from wind, solar energy or other fitful renewable energy resources. Combining nov...Electrolytic water splitting has been considered as a promising technology to produce highly pure H2 by using electrical power produced from wind, solar energy or other fitful renewable energy resources. Combining novel self-supporting structure and high-performance transition metal phosphides （TMP） shows substantial promise for practical application in water splitting. In this review, we try to provide a comprehensive analysis of the design and fabrication of various self-supported TMP electrodes for hydrogen evolution reaction, which are divided into three categories： catalysts growing on carbon-based substrates, catalysts growing on metal-based substrates and free- standing catalyst films. The material structures together with catalytic performances of self-supported electrodes are presented and discussed. We also show the specific strategies to further improve the catalytic performance by elemental doping or incorporation of nanocarbons. The simple and one-step methods to fabricate self-supported TMP electrodes are also highlighted. Finally, the chal- lenges and perspectives for self-supported TMP electrodes in water splitting application are briefly discussed.展开更多
Owing to stable spatial framework and large electrochemical interface,self-supported transition metal chalcogenides have been actively explored in renewable energy fields,especially in oxygen evolution reaction(OER).H...Owing to stable spatial framework and large electrochemical interface,self-supported transition metal chalcogenides have been actively explored in renewable energy fields,especially in oxygen evolution reaction(OER).Here,we review the research progress of self-supported transition metal chalcogenides(including sulfides,selenides,and tellurides)for the OER in recent years.The basic principle and evaluation parameters of OER are first introduced,and then the preparation methods of transition metal chalcogenides on various self-supporting substrates(including Ni foam(NF),carbon cloth(CC),carbon fiber paper(CFP),metal mesh/plate,etc.)are systematically summarized.Subsequently,advanced optimization strategies(including interface and defect engineering,heteroatom doping,edge engineering,surface morphology engineering,and construction of heterostructure)are introduced in detail to improve the inherent catalytic activity of self-supported electrocatalysts.Finally,the challenges and prospects of developing more promising self-supported chalcogenide electrocatalysts are proposed.展开更多
Scalable production of earth-abundant, easy-to-prepare, and cost-effective electrocatalysts for the hydrogen evolution reaction （HER） is essential for sustainable energy-based systems. Herein, we systematically stud...Scalable production of earth-abundant, easy-to-prepare, and cost-effective electrocatalysts for the hydrogen evolution reaction （HER） is essential for sustainable energy-based systems. Herein, we systematically studied the electrocatalytic HER performance of a self-supported ternary Co0.5Mn0.5P/carbon cloth （CC） nanomaterial prepared using a hydrothermal reaction and phosphorizafion process. Electrochemical tests demonstrated that the ternary Co0.5Mn0.5P/CC nanomaterial could be a highly active electrocatalyst in acidic media, with overpotentials of only 41 and 89 mV, affording current densities of 10 and 100 mA.cm-2, respectively, and a Tafel slope of 41.7 mV.dec-1. Furthermore, the electrocatalyst exhibited superior stability, with 3,000 cycles of cyclic voltammetry from -0.2 to 0.2 V at a scan rate of 100 mV.s-1 and 40 h of static polarization at a fixed overpotential of large-scale hydrogen production. 83 mV, indicating its potential for展开更多
The advancement of next-generation energy technologies calls for rationally designed and fabricated electrode materials that have desirable structures and satisfactory performance.Three-dimensional(3D)self-supported a...The advancement of next-generation energy technologies calls for rationally designed and fabricated electrode materials that have desirable structures and satisfactory performance.Three-dimensional(3D)self-supported amorphous nanomaterials have attracted great enthusiasm as the cornerstone for building high-performance nanodevices.In particular,tremendous efforts have been devoted to the design,fabrication,and evaluation of self-supported amorphous nanomaterials as electrodes for energy storage and conversion devices in the past decade.However,the electrochemical performance of devices assembled with 3D self-supported amorphous nanomaterials still remains to be dramatically promoted to satisfy the demands for more practical applications.In this review,we aim to outline the achievements made in recent years in the development of 3D self-supported amorphous nanomaterials for a broad range of energy storage and conversion processes.We firstly summarize different synthetic strategies employed to synthesize 3D nanomaterials and to tailor their composition,morphology,and structure.Then,the performance of these 3D self-supported amorphous nanomaterials in their corresponding energy-related reactions is highlighted.Finally,we draw out our comprehensive understanding towards both challenges and prospects of this promising field,where valuable guidance and inspiration will surely facilitate further development of 3D self-supported amorphous nanomaterials,thus enabling more highly efficient energy storage and conversion devices that play a key role in embracing a sustainable energy future.展开更多
The advancement of electrocatalytic N2 reduction reaction (NRR) toward ambient NH3 synthesis lies in the development of more affordable electrocatalysts than noble metals. Recently, various nanostructures of transitio...The advancement of electrocatalytic N2 reduction reaction (NRR) toward ambient NH3 synthesis lies in the development of more affordable electrocatalysts than noble metals. Recently, various nanostructures of transition metal compounds have been proposed as effective electrocatalysts;however, they exist in the form of loose powders, which have to be immobilized on a matrix before serving as the electrode for electrolysis. The matrix, being it carbon paper, carbon cloth or metal foam, is electrocatalytically inactive, whose introduction inevitably raises the invalid weight while sacrificing the active sites of the electrode. Herein, we report on the fabrication of a flexible ZrO2 nanofibrous membrane as a novel, self-supported electrocatalyst. The heteroatom doping can not only endow the nanofibrous membrane with excellent flexibility, but also induce oxygen vacancies which are responsible for easier adsorption of N2 on the ZrO2 surface. To improve the electrocatalytic activity, a facile SILAR approach is employed to decorate it with CdS quantum dots (QDs), thereby tuning its Fermi level. To improve the conductivity, a g-C3N4 nanolayer is further deposited which is both conductive and active. The resulting hierarchically structured, self-supported electrocatalyst, consisting of g-C3N4 encapsulated ZrO2 nanofibrous membrane decorated with CdS QDs, integrates the merits of the three components, and exhibits a remarkable synergy toward NRR. Excellent NH3 yield of 6.32 × 10−10 mol·s−1cm−2 (−0.6 V vs. RHE) and Faradaic efficiency of 12.9% (−0.4 V vs. RHE) are attained in 0.1 M Na2SO4.展开更多
Electrode materials are of decisive importance in determining the performance of electrochemical energy storage(EES)devices.Typically,the electrode materials are physically mixed with polymer binders and conductive ad...Electrode materials are of decisive importance in determining the performance of electrochemical energy storage(EES)devices.Typically,the electrode materials are physically mixed with polymer binders and conductive additives,which are then loaded on the current collectors to function in real devices.Such a configuration inevitably reduces the content of active species and introduces quite some undesired interfaces that bring down the energy densities and power capabilities.One viable solution to address this issue is to construct self-supported electrodes where the active species,for example transition metal oxides(TMOs),are directly integrated with conductive substrates without polymer binders and conductive additives.In this review,the recent progress of self-supported TMO-based electrodes for EES devices including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs),aluminum-ion batteries(AIBs),metal-air batteries,and supercapacitors(SCs),is discussed in great detail.The focused attention is firstly concentrated on their structural design and controllable synthesis.Then,the mechanism understanding of the enhanced electrochemical performance is presented.Finally,the challenges and prospects of self-supported TMO-based electrodes are summarized to end this review.展开更多
Tungsten carbide(WC)-based materials are widely considered as the hydrogen evolution reaction(HER)process catalysts due to their“Pt-like”electronic structure.Nonetheless,traditional powder electrodes have a high cos...Tungsten carbide(WC)-based materials are widely considered as the hydrogen evolution reaction(HER)process catalysts due to their“Pt-like”electronic structure.Nonetheless,traditional powder electrodes have a high cost,and display problems related to the process itself and the poor stability over operation time.This paper presented a self-supported asymmetric porous ceramic electrode with WO_(3-x)whiskers formed in situ on the walls of the finger-like holes and membrane surface,which was prepared by combining phase inversion tape-casting,pressureless sintering,and thermal treatment in a CO_(2) atmosphere.The optimized ceramic electrode displayed good catalytic HER activity and outstanding stability at high current densities.More specifically,it demonstrated the lowest overpotentials of 107 and 123 mV and the lowest Tafel slopes of 59.3 and 72.4 mV·dec^(-1)at 10 mA·cm^(-2)in acidic and alkaline media,respectively.This superior performance was ascribed to the structure of the ceramic membrane and the charge transfer efficiency,which was favored by the in situ developed WC/WO_(3-x)heterostructure and the oxygen vacancies.展开更多
Murdochite-type Ni6MnO8 three-dimensional mesoporous nanosheet arrays grown on carbon cloth （NMO-SA/CC） are synthesized using an in-situ growth strategy. As self-supported binder-free anodes for LIBs, the NMO-SA/CC ...Murdochite-type Ni6MnO8 three-dimensional mesoporous nanosheet arrays grown on carbon cloth （NMO-SA/CC） are synthesized using an in-situ growth strategy. As self-supported binder-free anodes for LIBs, the NMO-SA/CC hierarchical nanostructures exhibit ultrahigh capacity, excellent cycling stability, and good rate capability. The excellent lithium storage performance can be ascribed to the perfect electrical contact between NMO-SA and CC. The mesopores in the thin nanosheet can maximize the electrode contact with the electrolyte by decreasing the Li＋ diffusion path. Moreover, these effects relieve the pulverization and agglomeration that originate from the large volume variations during the Li＋ intercalation/deintercalation cycles. The in-situ X-ray absorption fine structure （XAFS） spectrum recorded during the initial lithiation/delithiation processes reveals the conversion reaction process.展开更多
Hard carbon stands out as the most promising candidate for anodes in sodium-ion battery.Nevertheless,addressing the challenges of low initial Coulombic efficiency and rate performance is crucial for practical applicat...Hard carbon stands out as the most promising candidate for anodes in sodium-ion battery.Nevertheless,addressing the challenges of low initial Coulombic efficiency and rate performance is crucial for practical applications.In this study,we employed a dimensionally designed approach,using six different biomass precursors,to preserve their inherent fine hierarchical morphological structures and appearances during the synthesis of selfsupporting carbon materials.Benefiting from its low-tortuosity structure that facilitates electron and ion transport,as well as its surface-enriched C=O functional groups and significant closed micropore areas,the obtained carbon material exhibits excellent electrochemical performance in sodium-ion storage,demonstrated by finite element simulation.Notably,the carbonized basswood exhibited a remarkable initial Coulombic efficiency of up to 92.4%and demonstrated outstanding rate performance,achieving a capacity of 223.3 mAh·g^(-1)at a high current density of2 A·g^(-1).In addition,thorough investigation was conducted on the influence of microstructure on the sodium storage behavior of hard carbon.Ex situ X-ray diffraction(XRD)was used to confirm that the capacity in the plateau region originates from interlayer insertion and closed-pore filling,which is consistent with the results obtained from smallangle X-ray scattering.These findings underscore the immense potential of leveraging surface functionalization and structural design to bolster the performance of hard carbon,paving the way for promising future advancements in this field.展开更多
High/medium entropy alloys(HEAs/MEAs)with high electrocatalytic activity have attracted great attention in water electrolysis applications.However,facile synthesis of self-supporting high/medium entropy alloys electro...High/medium entropy alloys(HEAs/MEAs)with high electrocatalytic activity have attracted great attention in water electrolysis applications.However,facile synthesis of self-supporting high/medium entropy alloys electrocatalysts with rich active sites through classical metallurgical methods is still a challenge.Here,a self-supporting porous FeCoNi MEA electrocatalyst with nanosheets-shaped surface for oxygen evolution reaction(OER)was prepared by a one-step electrochemical process from the metal oxides in molten CaCl_(2).The formation of the FeCoNi MEA is attributed to the oxides electro-reduction,high-temperature diffusion and solid solution.Additionally,the morphology and structure of the FeCoNi MEA can be precisely controlled by adjusting the electrolysis time and temperature.The electronic structure regulation and the reduced energy barrier of OER from the“cocktail effect”,the abundant exposed active sites brought by surface ultrathin nanosheets,the good electronic conductivity and electrochemical stability from the self-supporting structure enable the FeCoNi MEA electrode shows high-performance OER electrocatalysis,exhibiting a low overpotential of 233 mV at a current density of 10 mA cm^(-2),a low Tafel slope of 29.8 mV dec^(-1),and an excellent stability for over 500 h without any obvious structural destruction.This work demonstrates a facile one-step electrochemical metallurgical approach for fabricating self-supporting HEAs/MEAs electrocatalysts with nanosized surface for the application in water electrolysis.展开更多
Flexible electrode design with robust structure and good performance is one of the priorities for flexible batteries to power emerging wearable electronics,and organic cathode materials have become contenders for flex...Flexible electrode design with robust structure and good performance is one of the priorities for flexible batteries to power emerging wearable electronics,and organic cathode materials have become contenders for flexible self-supporting electrodes.However,issues such as easy electrolyte solubility and low intrinsic conductivity contribute to high polarization and rapid capacity decay.Herein,we have designed a flexible self-supporting cathode based on perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA),interfacial engineering enhanced by polypyrrole(PPy),and carbon nanotubes(CNTs),forming the interconnected and flexible PTCDA/PPy/CNTs using polymerization reaction and vacuum filtration methods,effectively curbing those challenges.When used as the cathode of sodium-ion batteries,PTCDA/PPy/CNTs exhibit excellent rate capability(105.7 mAh g^(−1) at 20 C),outstanding cycling stability(79.4%capacity retention at 5 C after 500 cycles),and remarkable wide temperature application capability(86.5 mAh g^(−1) at−30℃ and 115.4 mAh g^(−1) at 60℃).The sodium storage mechanism was verified to be a reversible oxidation reaction between two Na+ions and carbonyl groups by density functional theory calculations,in situ infrared Fourier transform infrared spectroscopy,and in situ Raman spectroscopy.Surprisingly,the pouch cells based on PTCDA/PPy/CNTs exhibit good mechanical flexibility in various mechanical states.This work inspires more rational designs of flexible and self-supporting organic cathodes,promoting the development of high-performance and wide-temperature adaptable wearable electronic devices.展开更多
The excess emission of nitrate from human activities disturbs the global nitrogen cycle and thus needs to be remediated.In this work,we prepared a La-doped Co_(3)O_(4)nanoneedle arrays catalyst for highly efficient el...The excess emission of nitrate from human activities disturbs the global nitrogen cycle and thus needs to be remediated.In this work,we prepared a La-doped Co_(3)O_(4)nanoneedle arrays catalyst for highly efficient electrocatalytic reduction of NO_(3)^(-) to NH_(3)at low concentration.The La-doped Co_(3)O_(4)nanoneedle arrays exhibit remarkable activity with the highest Faradaic efficiency of 95.5%and an ammonia yield rate of 4.08 mg/(h·cm^(2))at-0.3 V versus RHE in 0.02 mol/L NO_(3)^(-).Experiments and theoretical calculations show that the La doping not only facilitates the surface reconstruction to form active La-Co(OH)_(2),but also inhibits the hydrogen evolution reaction over Co sites,thus promoting the NH_(3)production.This work provides new insights into the promoting effect of the rare earth elements in transition metalbased electrocatalyst for nitrate reduction.展开更多
基金supported by the National Natural Science Foundation of China(22072107,21872105)the Natural Science Foundation of Shanghai(23ZR1464800)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Science&Technology Commission of Shanghai Municipality(19DZ2271500)。
文摘Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.
基金Tianjin Natural Science Foundation (23JCYBJC00660)Tianjin Enterprise Science and Technology Commissioner Project (23YDTPJC00490)+2 种基金National Natural Science Foundation of China (52203066, 51973157, 61904123)China Postdoctoral Science Foundation Grant (2023M742135)State Key Laboratory of Membrane and Membrane Separation, Tiangong University。
文摘Oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are the key reactions in numerous renewable energy devices. Unlike conventional powdered catalysts, self-supported catalysts are extensively employed in oxygen electrocatalysis because of the enhanced electron-transfer rate, high specific surface area, and superior mechanical flexibility. Among the self-supported conductive substrates, carbon fiber usually exhibits several distinctive advantages, such as a straightforward preparation process, relatively low cost, good stability, and excellent conductivity. Against this background,carbon fiber-based self-supported electrocatalysts have been widely applied and studied in oxygen electrocatalysis, indicating a promising development direction in oxygen electrocatalyst research.Thus, it is essential to offer an overall summary of the research progress in this field to facilitate its subsequent development. Taking the regulatory mechanisms and modification methods as a starting point, this review comprehensively summarizes recent research on carbon fiber-based self-supported electrocatalysts in recent years. Firstly, a brief overview of the synthesis methods and regulatory mechanisms of carbon fiber-based self-supported electrocatalysts is given. Furthermore, the view also highlights the modification methods and research progress of self-supported electrocatalysts synthesized on carbon fiber-based substrates in recent years in terms of different dopant atoms. Finally, the prospects for the application of self-supported electrocatalysts based on carbon fiber in oxygen electrocatalysis and the possible future directions of their development are presented. This review summarizes recent developments and applications of self-supported bi-functional electrocatalysts with carbon fiber-based materials as the conducting substrate in oxygen electrocatalysis. It also lays a robust scientific foundation for the subsequent reasonable design of highly effective carbon fiber-based self-supported electrocatalysts.
基金financially supported by the National Natural Science Foundation of China (Grants Nos. 51972349, U1801255 and 91963210)。
文摘To meet the practical demand of wearable/portable electronics, developing high-efficiency and durable multifunctional catalyst and in-situ assembling catalysts into electrodes with flexible features are urgently needed but challenging. Herein, we report a simple route to fabricate bendable multifunctional electrodes by in-situ carbonization of metal ion absorbed polyaniline precursor. Alloy nanoparticles encapsulated in graphite layer are uniformly distributed in the N-doping carbon nanorod skeleton. Profiting from the favorable free-standing structure and the cooperative effect of metallic nanoparticles, graphitic layer and N doped-carbon architecture, the trifunctional electrodes exhibit prominent activities and stability toward HER, OER and ORR. Notably, due to the protection of carbon layer, the electrocatalysts show the reversible catalytic HER/OER properties. The overall water splitting device can continuously work for 12 h under frequent exchanges of cathode and anode. Importantly, the bendable metal air batteries fabricated by self-supported electrode not only displays the outstanding battery performance,achieving a decent peak power density(125 mW cm^(-2)) and exhibiting favorable charge-discharge durability of 22 h, but also holds superb flexible stability. Specially, a lightweight self-driven water splitting unit is demonstrated with stable hydrogen production.
基金This research was supported by the Natural Science Foundation of China(52073295,51803226)the Sino-German Mobility Program(M-0424)+2 种基金Key Research Program of Frontier Sciences,Chinese Academy of Sciences(QYZDB-SSWSLH036)Bureau of International Cooperation,Chinese Academy of Sciences(174433KYSB20170061)K.C.Wong Education Foundation(GJTD-2019-13).
文摘Two-dimensional(2D)soft materials,especially in their self-supported forms,demonstrate attractive properties to realize biomimetic morphing and ultrasensitive sensing.Although extensive efforts on design of self-supported functional membranes and integrated systems have been devoted,there still remains an unexplored regime of the combination of mechanical,electrical and surface wetting properties for specific functions.Here,we report a self-supported film featured with elastic,thin,conductive and superhydrophobic characteristics.Through a well-defined surface modification strategy,the surface wettability and mechanical sensing can be effectively balanced.The resulted film can function as a smart umbrella to achieve real-time simulated raining with diverse frequencies and intensity.In addition,the integrated umbrella can even response sensitively to the sunlight and demonstrate a positively correlation of current signals with the intensity of sun illumination.Moreover,the superhydrophobic umbrella can be further employed to realize water rescue,which can take the underwater object onto water surface,load and rapidly transport the considerable weight.More importantly,the whole process of loaded objects and water flow velocity can be precisely detected.The self-supported smart umbrella can effectively monitor the weather and realize a smart water rescue,demonstrating significant potentials in multifunctional sensing and directional actuation in the presence of water.
基金Ministry of Higher Education(MOHE)Malaysia under the Fundamental Research Grant Scheme,Grant/Award Number:FRGS/1/2024/TK08/XMU/02/1PETRONAS-Academia Collaboration Dialogue(PACD 2023)grant+6 种基金Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF-APP NanoMalaysia BICEP Project 4,S.22015)National Natural Science Foundation of China,Grant/Award Number:22202168Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2021A1515111019Embassy of the People's Republic of China in Malaysia,Grant/Award Number:EENG/0045State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University,Grant/Award Number:2023X11Xiamen University Malaysia Investigatorship Grant,Grant/Award Number:IENG/0038Xiamen University Malaysia Research Fund,Grant/Award Numbers:ICOE/0001,XMUMRF/2021-C8/IENG/0041。
文摘Amid the ongoing transition toward renewable fuels,the self-supported layered double hydroxides(LDHs)are envisioned as propitious electrocatalysts for reinvigorating the electrocatalysis realm,thereby facilitating environmental remediation and bolstering sustainable global energy security.Exploiting appealing attributes such as unique lamellar structure,abundant active sites,tunable intercalation spacing and compositional flexibility,LDHs boast remarkable activity,selectivity and stability across diverse energy-related applications.By virtue of addressing the technological and time prominence of excavating their renaissance,this review first encompasses the facile state-of-the-art synthetic approaches alongside intriguing modification strategies,toward deciphering the authentic structure–performance correlations for advancing more robust and precise catalyst design.Aside from this,heterostructure engineering employing diversified ranges of coupling materials is highlighted,to construct ground-breaking binder-free LDHs-based heterostructures endowing with unprecedented activity and stability.Subsequently,the milestone gained from experimental research and theoretical modeling of this frontier in multifarious electrocatalytic applications,including HER,OER,UOR,AOR,seawater splitting and other fundamental conversion reactions is rigorously unveiled.As a final note,a brief conclusion is presented with an outline of future prospects.Essentially,this review aspires to offer enlightenment and incite wise inspiration for the future evolution of innovative and resilient next-generation catalysts.
基金supports provided by the National Natural Science Foundation of China(No.22202168)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515111019)+2 种基金This work was also funded by the Xiamen University Malaysia Investigatorship Grant(No.IENG/0038)the Xiamen University Malaysia Research Fund(Nos.ICOE/0001,XMUMRF/2021-C8/IENG/0041,and XMUMRF/2019-C3/IENG/0013)the Hengyuan International Sdn.Bhd.(No.EENG/0003).
文摘Hydrogen economy based on electrochemical water splitting exemplified one of the most promising means for overcoming the rapid consumption of fossil fuels and the serious deterioration of global climate.The development of earth-abundant,efficient,and durable electrocatalysts for hydrogen evolution reaction(HER)plays a vital role in the commercialization of water electrolysis.Regard,the self-supported electrode with unique nitrogen-doped reduced graphene oxide(N-rGO)nanoflakes and WS_(2) hierarchical nanoflower that were grown directly on carbon cloth(CC)substrate(WS_(2)/N-rGO/CC)was successfully synthesized using a facile dual-step hydrothermal approach.The as-synthesized 50%1T/2H-WS_(2)/N-rGO/CC(WGC),which possessed high metallic 1T phase of 57%not only efficiently exposed more active sites and accelerated mass/charge diffusion,but also endowed excellent structural lustiness,robust stability,and durability at a high current density.As a result,the 50%WGC exhibited lower overpotentials and Tafel slopes of 21.13 mV(29.55 mV∙dec^(-1))and 80.35 mV(137.02 mV∙dec^(-1))as compared to 20%Pt-C/CC,respectively for catalyzing acidic and alkaline hydrogen evolution reactions.Pivotally,the as-synthesized 50%WGC also depicted long-term stability for more than 8 h in the high-current-density regions(100 and 220 mA∙cm^(-2)).In brief,this work reveals a self-supported electrode as an extraordinary alternative to Pt-based catalysts for HER in a wide pH range,while paving a facile strategy to develop advanced electrocatalysts with abundant heterointerfaces for practical applications in energy-saving hydrogen production.
文摘WS2/carbon nanofibers （WS2/CNFs） are obtained by a simple electrospinning method in which few-/ single-layer WS2 is uniformly embedded in carbon fibers. When used as the active anode material for Li-ion cells, these nanofibers exhibit a first-cycle discharge/charge capacity of 941/756 mAh/g at 100 mAJg and maintain a capacity of 458 mAh/g after 100 cycles at 1 A/g. The evolution of size and crystallinity of WS2 with heating treatment are system- atically studied, which are found to strongly influence the final electrochemical performance. Interestingly, the WS2 samples of lowest crystallinity show the highest performance among all studied samples, which could result from the large interfacial capacity for Li ions due to their large specific surface area. More interestingly, the inherent flexible attribute of electrospun nanofibers renders them a great potential in the utilization of binder-flee anodes. Similar high discharge/charge capacity of 761/604 mAh/g with a first coulombic efficiency of 79.4 % has been achieved in these binder-flee anodes. Considering the universal of such simple and scalable preparation strategy, it is very likely to extend this method to other similar two-dimensional layered materials besides WS2 and provides a promising candidate elec- trode for developing flexible battery devices.
基金supported by the National Natural Science Foundation of China (21231005, 51231003)the Program of Introducing Talents of Discipline to Universities of China (B12015)
文摘Developing high-performance anode materials for potassium-ion batteries is significantly urgent. We here demonstrate Sb_2S_3 nanoparticles(~20 nm) homogeneously dispersed in porous S,N-codoped graphene framework(Sb_2S_3-SNG) as a self-supported anode material for potassium-ion batteries. The rational structure design of integrating Sb_2S_3 nanoparticles with S,N-codoped graphene contributes to high reactivity, strong affinity, good electric conductivity, and robust stability of the composite, enabling superior K-storage performance. Moreover, the self-supported architecture significantly decreases the inactive weight of the battery, resulting in a high energy density of a Sb_2S_3-SNG/KVPO_4 F-C full cell to ~166.3 W h kg^(-1).
文摘Electrolytic water splitting has been considered as a promising technology to produce highly pure H2 by using electrical power produced from wind, solar energy or other fitful renewable energy resources. Combining novel self-supporting structure and high-performance transition metal phosphides （TMP） shows substantial promise for practical application in water splitting. In this review, we try to provide a comprehensive analysis of the design and fabrication of various self-supported TMP electrodes for hydrogen evolution reaction, which are divided into three categories： catalysts growing on carbon-based substrates, catalysts growing on metal-based substrates and free- standing catalyst films. The material structures together with catalytic performances of self-supported electrodes are presented and discussed. We also show the specific strategies to further improve the catalytic performance by elemental doping or incorporation of nanocarbons. The simple and one-step methods to fabricate self-supported TMP electrodes are also highlighted. Finally, the chal- lenges and perspectives for self-supported TMP electrodes in water splitting application are briefly discussed.
基金This work was supported by the National Natural Science Foundation of China(No.22075099)the Natural Science Foundation of Jilin Province(No.20220101051JC)the Education Department of Jilin Province(No.JJKH20220967KJ).
文摘Owing to stable spatial framework and large electrochemical interface,self-supported transition metal chalcogenides have been actively explored in renewable energy fields,especially in oxygen evolution reaction(OER).Here,we review the research progress of self-supported transition metal chalcogenides(including sulfides,selenides,and tellurides)for the OER in recent years.The basic principle and evaluation parameters of OER are first introduced,and then the preparation methods of transition metal chalcogenides on various self-supporting substrates(including Ni foam(NF),carbon cloth(CC),carbon fiber paper(CFP),metal mesh/plate,etc.)are systematically summarized.Subsequently,advanced optimization strategies(including interface and defect engineering,heteroatom doping,edge engineering,surface morphology engineering,and construction of heterostructure)are introduced in detail to improve the inherent catalytic activity of self-supported electrocatalysts.Finally,the challenges and prospects of developing more promising self-supported chalcogenide electrocatalysts are proposed.
基金This project was supported by National Natural Science Foundation of China （No. 21190040）.
文摘Scalable production of earth-abundant, easy-to-prepare, and cost-effective electrocatalysts for the hydrogen evolution reaction （HER） is essential for sustainable energy-based systems. Herein, we systematically studied the electrocatalytic HER performance of a self-supported ternary Co0.5Mn0.5P/carbon cloth （CC） nanomaterial prepared using a hydrothermal reaction and phosphorizafion process. Electrochemical tests demonstrated that the ternary Co0.5Mn0.5P/CC nanomaterial could be a highly active electrocatalyst in acidic media, with overpotentials of only 41 and 89 mV, affording current densities of 10 and 100 mA.cm-2, respectively, and a Tafel slope of 41.7 mV.dec-1. Furthermore, the electrocatalyst exhibited superior stability, with 3,000 cycles of cyclic voltammetry from -0.2 to 0.2 V at a scan rate of 100 mV.s-1 and 40 h of static polarization at a fixed overpotential of large-scale hydrogen production. 83 mV, indicating its potential for
基金This work was supported by the National Natural Science Foundation of China(Nos.52272181,51872016,and 52201261)China Postdoctoral Science Foundation(Nos.2020TQ0023 and 2020M680295).
文摘The advancement of next-generation energy technologies calls for rationally designed and fabricated electrode materials that have desirable structures and satisfactory performance.Three-dimensional(3D)self-supported amorphous nanomaterials have attracted great enthusiasm as the cornerstone for building high-performance nanodevices.In particular,tremendous efforts have been devoted to the design,fabrication,and evaluation of self-supported amorphous nanomaterials as electrodes for energy storage and conversion devices in the past decade.However,the electrochemical performance of devices assembled with 3D self-supported amorphous nanomaterials still remains to be dramatically promoted to satisfy the demands for more practical applications.In this review,we aim to outline the achievements made in recent years in the development of 3D self-supported amorphous nanomaterials for a broad range of energy storage and conversion processes.We firstly summarize different synthetic strategies employed to synthesize 3D nanomaterials and to tailor their composition,morphology,and structure.Then,the performance of these 3D self-supported amorphous nanomaterials in their corresponding energy-related reactions is highlighted.Finally,we draw out our comprehensive understanding towards both challenges and prospects of this promising field,where valuable guidance and inspiration will surely facilitate further development of 3D self-supported amorphous nanomaterials,thus enabling more highly efficient energy storage and conversion devices that play a key role in embracing a sustainable energy future.
基金This work was financially supported by the Fundamental Research Funds for the Central Universities(No.2232019G-01)the National Natural Science Foundation of China(Nos.21961132024,51925302 and 51873029)+3 种基金the Natural Science Foundation of Shanghai(No.19ZR1401100)the Innovation Program of Shanghai Municipal Education Commission(No.2017-01-07-00-03-E00024)the Program of Shanghai Academic Research Leader(No.18XD1400200)the DHU Distinguished Young Professor Program(No.LZA2020001).
文摘The advancement of electrocatalytic N2 reduction reaction (NRR) toward ambient NH3 synthesis lies in the development of more affordable electrocatalysts than noble metals. Recently, various nanostructures of transition metal compounds have been proposed as effective electrocatalysts;however, they exist in the form of loose powders, which have to be immobilized on a matrix before serving as the electrode for electrolysis. The matrix, being it carbon paper, carbon cloth or metal foam, is electrocatalytically inactive, whose introduction inevitably raises the invalid weight while sacrificing the active sites of the electrode. Herein, we report on the fabrication of a flexible ZrO2 nanofibrous membrane as a novel, self-supported electrocatalyst. The heteroatom doping can not only endow the nanofibrous membrane with excellent flexibility, but also induce oxygen vacancies which are responsible for easier adsorption of N2 on the ZrO2 surface. To improve the electrocatalytic activity, a facile SILAR approach is employed to decorate it with CdS quantum dots (QDs), thereby tuning its Fermi level. To improve the conductivity, a g-C3N4 nanolayer is further deposited which is both conductive and active. The resulting hierarchically structured, self-supported electrocatalyst, consisting of g-C3N4 encapsulated ZrO2 nanofibrous membrane decorated with CdS QDs, integrates the merits of the three components, and exhibits a remarkable synergy toward NRR. Excellent NH3 yield of 6.32 × 10−10 mol·s−1cm−2 (−0.6 V vs. RHE) and Faradaic efficiency of 12.9% (−0.4 V vs. RHE) are attained in 0.1 M Na2SO4.
基金This work was finally supported by the National Nature Science Foundation of China(Grant No.21975287)the start-up funding support of China University of Petroleum(East China),Taishan Scholar Project(Grant No.ts201712020)+1 种基金Technological Leading Scholar of 10000 Talent Project(Grant No.W03020508)Shandong Provincial Natural Science Foundation(Grant No.ZR2018ZC1458).
文摘Electrode materials are of decisive importance in determining the performance of electrochemical energy storage(EES)devices.Typically,the electrode materials are physically mixed with polymer binders and conductive additives,which are then loaded on the current collectors to function in real devices.Such a configuration inevitably reduces the content of active species and introduces quite some undesired interfaces that bring down the energy densities and power capabilities.One viable solution to address this issue is to construct self-supported electrodes where the active species,for example transition metal oxides(TMOs),are directly integrated with conductive substrates without polymer binders and conductive additives.In this review,the recent progress of self-supported TMO-based electrodes for EES devices including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs),aluminum-ion batteries(AIBs),metal-air batteries,and supercapacitors(SCs),is discussed in great detail.The focused attention is firstly concentrated on their structural design and controllable synthesis.Then,the mechanism understanding of the enhanced electrochemical performance is presented.Finally,the challenges and prospects of self-supported TMO-based electrodes are summarized to end this review.
基金This research was supported by the National Natural Science Foundation of China(U1732115)the China National Petroleum Corporation(KD200121)+1 种基金the Science and Technology Department of Henan Province(222102230054)the Henan Province Education Department of Key Scientific Research Project in Colleges and Universities(21B430012).
文摘Tungsten carbide(WC)-based materials are widely considered as the hydrogen evolution reaction(HER)process catalysts due to their“Pt-like”electronic structure.Nonetheless,traditional powder electrodes have a high cost,and display problems related to the process itself and the poor stability over operation time.This paper presented a self-supported asymmetric porous ceramic electrode with WO_(3-x)whiskers formed in situ on the walls of the finger-like holes and membrane surface,which was prepared by combining phase inversion tape-casting,pressureless sintering,and thermal treatment in a CO_(2) atmosphere.The optimized ceramic electrode displayed good catalytic HER activity and outstanding stability at high current densities.More specifically,it demonstrated the lowest overpotentials of 107 and 123 mV and the lowest Tafel slopes of 59.3 and 72.4 mV·dec^(-1)at 10 mA·cm^(-2)in acidic and alkaline media,respectively.This superior performance was ascribed to the structure of the ceramic membrane and the charge transfer efficiency,which was favored by the in situ developed WC/WO_(3-x)heterostructure and the oxygen vacancies.
基金Acknowledgements We gratefully acknowledge the support of this research by the National Natural Science Foundation of China （Nos. 21371053, 21376065, 21401048, and 21571054）, the Postdoctoral Science Foundation of Heilongjiang Province （No. LBH-TZ0519）, Harbin Science and Technology Innovation Talents Research Foundation （No. 2015RAQXJ057）, Innovative Research Project of Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education.
文摘Murdochite-type Ni6MnO8 three-dimensional mesoporous nanosheet arrays grown on carbon cloth （NMO-SA/CC） are synthesized using an in-situ growth strategy. As self-supported binder-free anodes for LIBs, the NMO-SA/CC hierarchical nanostructures exhibit ultrahigh capacity, excellent cycling stability, and good rate capability. The excellent lithium storage performance can be ascribed to the perfect electrical contact between NMO-SA and CC. The mesopores in the thin nanosheet can maximize the electrode contact with the electrolyte by decreasing the Li＋ diffusion path. Moreover, these effects relieve the pulverization and agglomeration that originate from the large volume variations during the Li＋ intercalation/deintercalation cycles. The in-situ X-ray absorption fine structure （XAFS） spectrum recorded during the initial lithiation/delithiation processes reveals the conversion reaction process.
基金financially supported by the National Natural Science Foundation of China(Nos.32171709 and 32271791)China Postdoctoral Science Foundation(No.2023M743972)。
文摘Hard carbon stands out as the most promising candidate for anodes in sodium-ion battery.Nevertheless,addressing the challenges of low initial Coulombic efficiency and rate performance is crucial for practical applications.In this study,we employed a dimensionally designed approach,using six different biomass precursors,to preserve their inherent fine hierarchical morphological structures and appearances during the synthesis of selfsupporting carbon materials.Benefiting from its low-tortuosity structure that facilitates electron and ion transport,as well as its surface-enriched C=O functional groups and significant closed micropore areas,the obtained carbon material exhibits excellent electrochemical performance in sodium-ion storage,demonstrated by finite element simulation.Notably,the carbonized basswood exhibited a remarkable initial Coulombic efficiency of up to 92.4%and demonstrated outstanding rate performance,achieving a capacity of 223.3 mAh·g^(-1)at a high current density of2 A·g^(-1).In addition,thorough investigation was conducted on the influence of microstructure on the sodium storage behavior of hard carbon.Ex situ X-ray diffraction(XRD)was used to confirm that the capacity in the plateau region originates from interlayer insertion and closed-pore filling,which is consistent with the results obtained from smallangle X-ray scattering.These findings underscore the immense potential of leveraging surface functionalization and structural design to bolster the performance of hard carbon,paving the way for promising future advancements in this field.
基金supported by the National Natural Science Foundation of China(Nos.52022054,51974181,52004155,52004157,52374307,52304331,52334009)the National Key Research and Development Program of China(No.2022YFC2906100)+4 种基金the China Postdoctoral Science Foundation(No.2022M712023)the Science and Technology Commission of Shanghai Municipality(No.21DZ1208900)the Innovation Program of Shanghai Municipal Education Commission(No.2023ZKZD48)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning(No.TP2019041)the“Shuguang Program”supported by the Shanghai Education Development Foundation and the Shanghai Municipal Education Commission(No.21SG42).
文摘High/medium entropy alloys(HEAs/MEAs)with high electrocatalytic activity have attracted great attention in water electrolysis applications.However,facile synthesis of self-supporting high/medium entropy alloys electrocatalysts with rich active sites through classical metallurgical methods is still a challenge.Here,a self-supporting porous FeCoNi MEA electrocatalyst with nanosheets-shaped surface for oxygen evolution reaction(OER)was prepared by a one-step electrochemical process from the metal oxides in molten CaCl_(2).The formation of the FeCoNi MEA is attributed to the oxides electro-reduction,high-temperature diffusion and solid solution.Additionally,the morphology and structure of the FeCoNi MEA can be precisely controlled by adjusting the electrolysis time and temperature.The electronic structure regulation and the reduced energy barrier of OER from the“cocktail effect”,the abundant exposed active sites brought by surface ultrathin nanosheets,the good electronic conductivity and electrochemical stability from the self-supporting structure enable the FeCoNi MEA electrode shows high-performance OER electrocatalysis,exhibiting a low overpotential of 233 mV at a current density of 10 mA cm^(-2),a low Tafel slope of 29.8 mV dec^(-1),and an excellent stability for over 500 h without any obvious structural destruction.This work demonstrates a facile one-step electrochemical metallurgical approach for fabricating self-supporting HEAs/MEAs electrocatalysts with nanosized surface for the application in water electrolysis.
基金Shuangqiang Chen gratefully acknowledges the NationalNatural Science Foundation ofChina(21975154,22179078)Zhejiang Provincial Natural Science Founda-tion of China(LY24E020002)+3 种基金Shanghai MunicipalEducation Commission(Innovation Program:2019-01-07-00-09-E00021)the Innovative Research Team of High-level Local Universities in Shanghai.Bing Sunwould like to thank the financial support from ARCthrough the ARC Future Fellowship(FT220100561)YaoXiao would like to thank the financial support from theNatural Science Foundation of Zhejiang Province(LQ23E020002)the Wenzhou Key Scientific andTechnological Innovation Research Project(ZG2023053)
文摘Flexible electrode design with robust structure and good performance is one of the priorities for flexible batteries to power emerging wearable electronics,and organic cathode materials have become contenders for flexible self-supporting electrodes.However,issues such as easy electrolyte solubility and low intrinsic conductivity contribute to high polarization and rapid capacity decay.Herein,we have designed a flexible self-supporting cathode based on perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA),interfacial engineering enhanced by polypyrrole(PPy),and carbon nanotubes(CNTs),forming the interconnected and flexible PTCDA/PPy/CNTs using polymerization reaction and vacuum filtration methods,effectively curbing those challenges.When used as the cathode of sodium-ion batteries,PTCDA/PPy/CNTs exhibit excellent rate capability(105.7 mAh g^(−1) at 20 C),outstanding cycling stability(79.4%capacity retention at 5 C after 500 cycles),and remarkable wide temperature application capability(86.5 mAh g^(−1) at−30℃ and 115.4 mAh g^(−1) at 60℃).The sodium storage mechanism was verified to be a reversible oxidation reaction between two Na+ions and carbonyl groups by density functional theory calculations,in situ infrared Fourier transform infrared spectroscopy,and in situ Raman spectroscopy.Surprisingly,the pouch cells based on PTCDA/PPy/CNTs exhibit good mechanical flexibility in various mechanical states.This work inspires more rational designs of flexible and self-supporting organic cathodes,promoting the development of high-performance and wide-temperature adaptable wearable electronic devices.
基金Project supported by the National Natural Science Foundation of China(21971129,21961022,21661023)the Inner Mongolia Autonomous Region 2022 Leading Talent Team of Science and Technology(2022LJRC0008)+5 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2022MS02014,2021BS02007)the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region(NJYT23031)the 111 Project(D20033)the"Grassland Leading Talent"Program of Inner Mongoliathe"Grassland-Talent"Innovation Team of Inner Mongoliathe"Science and Technology for A Better Development of Inner Mongolia"Program(2020XM03)。
文摘The excess emission of nitrate from human activities disturbs the global nitrogen cycle and thus needs to be remediated.In this work,we prepared a La-doped Co_(3)O_(4)nanoneedle arrays catalyst for highly efficient electrocatalytic reduction of NO_(3)^(-) to NH_(3)at low concentration.The La-doped Co_(3)O_(4)nanoneedle arrays exhibit remarkable activity with the highest Faradaic efficiency of 95.5%and an ammonia yield rate of 4.08 mg/(h·cm^(2))at-0.3 V versus RHE in 0.02 mol/L NO_(3)^(-).Experiments and theoretical calculations show that the La doping not only facilitates the surface reconstruction to form active La-Co(OH)_(2),but also inhibits the hydrogen evolution reaction over Co sites,thus promoting the NH_(3)production.This work provides new insights into the promoting effect of the rare earth elements in transition metalbased electrocatalyst for nitrate reduction.
