以氯化钴、对叔丁基磺酰杯[4]芳烃(H4TC4A-SO2)和非对称性3-(1H-四唑-5-基)苯甲酸(H2L)为原料,通过溶剂热法合成了一个具有四面体配位笼结构的16核化合物[Co16(TC4A-SO2)4(OH)4(L)8]·[(C8H20N)(C4H12N)2(C2H8N)]·solvent(Co16...以氯化钴、对叔丁基磺酰杯[4]芳烃(H4TC4A-SO2)和非对称性3-(1H-四唑-5-基)苯甲酸(H2L)为原料,通过溶剂热法合成了一个具有四面体配位笼结构的16核化合物[Co16(TC4A-SO2)4(OH)4(L)8]·[(C8H20N)(C4H12N)2(C2H8N)]·solvent(Co16-TC4A-SO2).采用X射线单晶衍射、X射线粉末衍射、热重分析、红外光谱方法对配合物进行了表征.将Co16-TC4A-SO2笼簇直接负载到碳纸上(Co16-TC4A-SO2/CP)用作工作电极,其对析氧反应(OER)展现出较好的催化性能.在1 mol/L KOH中,Co16-TC4A-SO2/CP在343.8 m V的过电位下达到10.0 m A/cm^2电流密度,Tafel斜率为79.31 m V/dec,并且在20.0 m A/cm2电流密度下表现出长达48 h的催化稳定性.展开更多
Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then...Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).展开更多
Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water split...Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water splitting electrolysis.However,noble metal-based catalysts often suffer from multiple disadvantages,including high cost,low selectivity and poor durability.The emergence of metal-organic framework nanosheets(MOFNSs)attracts significant attention due to their unique advantages.Here,a concise,yet comprehensive and critical,review of recent advances in the field of MOFNSs is provided.This review explains the fundamental oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed.Moreover,it discusses efficient design strategies and the brief research advances of MOFNSs in HER,OER,and bifunctional electrocatalysis,along with some challenges and opportunities.展开更多
With the goal of constructing a carbon‐free energy cycle,proton‐exchange membrane(PEM)water electrolysis is a promising technology that can be integrated effectively with renewable energy resources to produce high‐...With the goal of constructing a carbon‐free energy cycle,proton‐exchange membrane(PEM)water electrolysis is a promising technology that can be integrated effectively with renewable energy resources to produce high‐purity hydrogen.IrO2,as a commercial electrocatalyst for the anode side of a PEM water electrolyzer,can both overcome the high corrosion conditions and exhibit efficient catalytic performance.However,the high consumption of Ir species cannot meet the sustainable development and economic requirements of this technology.Accordingly,it is necessary to understand the OER catalytic mechanisms for Ir species,further designing new types of low‐iridium catalysts with high activity and stability to replace IrO2.In this review,we first summarize the related catalytic mechanisms of the acidic oxygen evolution reaction(OER),and then provide general methods for measuring the catalytic performance of materials.Second,we present the structural evolution results of crystalline IrO2 and amorphous IrOx using in situ characterization techniques under catalytic conditions to understand the common catalytic characteristics of the materials and the possible factors affecting the structural evolution characteristics.Furthermore,we focus on three types of common low‐iridium catalysts,including heteroatom‐doped IrO2(IrOx)‐based catalysts,perovskite‐type iridium‐based catalysts,and pyrochlore‐type iridium‐based catalysts,and try to correlate the structural features with the intrinsic catalytic performance of materials.Finally,at the end of the review,we present the unresolved problems and challenges in this field in an attempt to develop effective strategies to further balance the catalytic activity and stability of materials under acidic OER catalytic conditions.展开更多
The oxygen evolution reaction(OER)plays an important role in the development of energy conversation and storage technologies including water splitting and metal-air batteries,where the development of electrocatalysts ...The oxygen evolution reaction(OER)plays an important role in the development of energy conversation and storage technologies including water splitting and metal-air batteries,where the development of electrocatalysts is paramount.In this study,cobalt-nickel phosphide/N-doped porous carbon polyhedron electrocatalysts(CoNiP/NC)were prepared by a facile two-step carbonization method and subsequent phosphorization calcination in an Ar atmosphere using cobalt-based zeolitic imidazolate frameworks(ZIFs)as precursors.Among the electrocatalysts obtained by controlling the carbonization and phosphorization temperature,the CoNiP/NC700 catalyst,where 700 refers to the calcination temperature(°C),exhibited superior electrocatalytic activity for the OER with an onset overpotential of approximate 220 mV and an overpotential of approximate 300 mV in alkaline solution at a current density of 10 mA/cm2.The CoNi/NC and Co/NC Samples were also tested for comparison and CoNiP/NC exhibited the better electrocatalytic activity at all the temperatures tested.The superior electrocatalytic activity of the phosphorization hybrid material can be attributed to the superior synergistic effect of Co,Ni,P and C due to their strong electron coupling interactions.The interconnected amorphous carbon anchored the active Co compounds to avoid aggregation and maintained conducting channels for electron transfer.The composite electrocatalyst prepared herein is a promising candidate for use in electrocatalytic OERs.展开更多
Nanowires with anisotropic morphologies have been applied in various scientific and technological areas.It is also widely employed to fabricate nanowires into high-dimensional superstructures(arrays,networks etc.)to o...Nanowires with anisotropic morphologies have been applied in various scientific and technological areas.It is also widely employed to fabricate nanowires into high-dimensional superstructures(arrays,networks etc.)to overcome the shortcomings of low-dimensional nanowires.However,typical strategies for constructing these superstructures are restricted to complicated and harsh synthetic conditions,not to mention unique 3D structures with advanced properties beyond common superstructures.Herein,we report an unusual network ofα-MnO_(2)nanowires with structure-induced hydrophilicity and conductivity.In the network,the nanowires are interconnected from all directions by nodes,and the 3D network structure is formed from the endless connection of nodes in a node-by-node way.The unique network structure brings about high hydrophilicity and conductivity,both of which are positive factors for an efficient electrocatalyst.Accordingly,the α-MnO_(2) network was tested for electrocatalytic water oxidation and showed significantly enhanced activity compared with isolatedα-MnO_(2)nanowires and 3Dα-MnO_(2)microspheres.This study not only provides a synthetic route toward an advanced network structure but also a new idea for the design of materials for electrochemistry with both efficient mass diffusion and charge transfer.展开更多
Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OE...Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OER). In this work, triangular Cu@CuO nanorods on Cu nanosheets were fabricated by a novel in-situ oxidation approach using Cu nanosheets as self-template and conductive nano-substrate in an aqueous solution of NaOH/H2O2, and then by lowtemperature phosphorization treatments. The experimental results show that the phosphating temperature has a significant effect on the morphology, composition and number of active sites of Cu@Cu_(3)P nanorods. The Cu@Cu_(3)P-280 electrode exhibits a good HER catalytic activity of achieving a current density of 10 mA/cm^(2) at 252 mV in acid electrolyte. After catalysis for 14 h, the current density can still reach 72% of the initial value. Moreover, the Cu@Cu_(3)P-280 electrode also shows an excellent OER catalytic activity in basic electrolyte, reaching a current density of 10 mA/cm^(2) at the overpotential value of 200 mV. After catalysis for 12 h, the current density remained more than 93% of the initial value. This work provides a theoretical basis for the directional design and preparation of sustainable, low-cost, bifunctional electrocatalytic materials.展开更多
The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/...The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.展开更多
Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic o...Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic oxygen evolution reaction(OER)is still shortage.Herein,we report remarkable promotion of OER performance on the NiFe‐based nanocomposite electrocatalyst via the synergy of multiple carbon‐based interface engineering.Specifically,carbon nanotubes were in situ grown on carbon fiber paper to improve the interface between CFP and NiFeO_(x)H_(y),and graphite carbon nanoparticles were in situ loaded and partly doped into the NiFeO_(x)H_(y) to modify the intergranular interface charge transfer and electronic structure of NiFeO_(x)H_(y).Consequently,the as‐obtained NiFeO_(x)H_(y)‐C/CNTs/CFP catalyst exhibited significantly enhanced electrocatalytic OER activity with an overpotential of 202 mV at 10 mA cm^(-2) in 1 mol L^(-1) KOH.Our work not only extends application of carbon materials but also provides an alternative strategy to develop highly efficient electrocatalysts.展开更多
Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increa...Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increasing attention as active OER catalysts due to their excellent physical and chemical characters,and massive efforts have been devoted to improving the phosphide and sulfide‐based materials with better activity and stability in recent years.In this review,the recent progress on phosphide and sulfide‐based OER electrocatalysts in terms of chemical properties,synthetic methodologies,catalytic performances evaluation and improvement strategy is reviewed.The most accepted reaction pathways as well as the thermodynamics and electrochemistry of the OER are firstly introduced in brief,followed by a summary of the recent research and optimization strategy of phosphide and sulfide‐based OER electrocatalysts.Finally,some mechanistic studies of the active phase of phosphide and sulfide‐based compounds are discussed to give insight into the nature of active catalytic sites.It is expected to indicate guidance for further improving the performances of phosphide and sulfide‐based OER electrocatalysts.展开更多
Metal‐organic frameworks(MOFs)are a series of highly porous crystalline materials,which are built from inorganic metal nodes and organic linkers through coordination bonds.Their unique porous structural features(such...Metal‐organic frameworks(MOFs)are a series of highly porous crystalline materials,which are built from inorganic metal nodes and organic linkers through coordination bonds.Their unique porous structural features(such as high porosity,high surface areas,and highly ordered nanoporous structures)and designable structures and compositions have facilitated their use in gas capture,separation,catalysis,and energy storage and conversion.Recently,the design and synthesis of pure MOFs and their derivatives have opened new routes to develop highly efficient electrocatalysts toward oxygen reduction reactions(ORR)and oxygen evolution reactions(OER),which are the core electrode reactions in many energy storage and conversion techniques,such as metal‐air batteries and fuel cells.This review first discusses recent progress in the synthesis and the electrocatalytic applications of pure MOF‐based electrocatalysts toward ORR or OER,including pure MOFs,MOFs decorated with active species,and MOFs incorporated with conductive materials.The following section focuses on the advancements of the design and preparation of various MOF‐derived materials-such as inorganic nano‐(or micro‐)structures/porous carbon composites,pure porous carbons,pure inorganic nano‐(or micro‐)structured materials,and single‐atom electrocatalysts-and their applications in oxygen electrocatalysis.Finally,we present a conclusion and an outlook for some general design strategies and future research directions of MOF‐based oxygen electrocatalysts.展开更多
文摘以氯化钴、对叔丁基磺酰杯[4]芳烃(H4TC4A-SO2)和非对称性3-(1H-四唑-5-基)苯甲酸(H2L)为原料,通过溶剂热法合成了一个具有四面体配位笼结构的16核化合物[Co16(TC4A-SO2)4(OH)4(L)8]·[(C8H20N)(C4H12N)2(C2H8N)]·solvent(Co16-TC4A-SO2).采用X射线单晶衍射、X射线粉末衍射、热重分析、红外光谱方法对配合物进行了表征.将Co16-TC4A-SO2笼簇直接负载到碳纸上(Co16-TC4A-SO2/CP)用作工作电极,其对析氧反应(OER)展现出较好的催化性能.在1 mol/L KOH中,Co16-TC4A-SO2/CP在343.8 m V的过电位下达到10.0 m A/cm^2电流密度,Tafel斜率为79.31 m V/dec,并且在20.0 m A/cm2电流密度下表现出长达48 h的催化稳定性.
文摘Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).
文摘Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water splitting electrolysis.However,noble metal-based catalysts often suffer from multiple disadvantages,including high cost,low selectivity and poor durability.The emergence of metal-organic framework nanosheets(MOFNSs)attracts significant attention due to their unique advantages.Here,a concise,yet comprehensive and critical,review of recent advances in the field of MOFNSs is provided.This review explains the fundamental oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed.Moreover,it discusses efficient design strategies and the brief research advances of MOFNSs in HER,OER,and bifunctional electrocatalysis,along with some challenges and opportunities.
文摘With the goal of constructing a carbon‐free energy cycle,proton‐exchange membrane(PEM)water electrolysis is a promising technology that can be integrated effectively with renewable energy resources to produce high‐purity hydrogen.IrO2,as a commercial electrocatalyst for the anode side of a PEM water electrolyzer,can both overcome the high corrosion conditions and exhibit efficient catalytic performance.However,the high consumption of Ir species cannot meet the sustainable development and economic requirements of this technology.Accordingly,it is necessary to understand the OER catalytic mechanisms for Ir species,further designing new types of low‐iridium catalysts with high activity and stability to replace IrO2.In this review,we first summarize the related catalytic mechanisms of the acidic oxygen evolution reaction(OER),and then provide general methods for measuring the catalytic performance of materials.Second,we present the structural evolution results of crystalline IrO2 and amorphous IrOx using in situ characterization techniques under catalytic conditions to understand the common catalytic characteristics of the materials and the possible factors affecting the structural evolution characteristics.Furthermore,we focus on three types of common low‐iridium catalysts,including heteroatom‐doped IrO2(IrOx)‐based catalysts,perovskite‐type iridium‐based catalysts,and pyrochlore‐type iridium‐based catalysts,and try to correlate the structural features with the intrinsic catalytic performance of materials.Finally,at the end of the review,we present the unresolved problems and challenges in this field in an attempt to develop effective strategies to further balance the catalytic activity and stability of materials under acidic OER catalytic conditions.
文摘The oxygen evolution reaction(OER)plays an important role in the development of energy conversation and storage technologies including water splitting and metal-air batteries,where the development of electrocatalysts is paramount.In this study,cobalt-nickel phosphide/N-doped porous carbon polyhedron electrocatalysts(CoNiP/NC)were prepared by a facile two-step carbonization method and subsequent phosphorization calcination in an Ar atmosphere using cobalt-based zeolitic imidazolate frameworks(ZIFs)as precursors.Among the electrocatalysts obtained by controlling the carbonization and phosphorization temperature,the CoNiP/NC700 catalyst,where 700 refers to the calcination temperature(°C),exhibited superior electrocatalytic activity for the OER with an onset overpotential of approximate 220 mV and an overpotential of approximate 300 mV in alkaline solution at a current density of 10 mA/cm2.The CoNi/NC and Co/NC Samples were also tested for comparison and CoNiP/NC exhibited the better electrocatalytic activity at all the temperatures tested.The superior electrocatalytic activity of the phosphorization hybrid material can be attributed to the superior synergistic effect of Co,Ni,P and C due to their strong electron coupling interactions.The interconnected amorphous carbon anchored the active Co compounds to avoid aggregation and maintained conducting channels for electron transfer.The composite electrocatalyst prepared herein is a promising candidate for use in electrocatalytic OERs.
文摘Nanowires with anisotropic morphologies have been applied in various scientific and technological areas.It is also widely employed to fabricate nanowires into high-dimensional superstructures(arrays,networks etc.)to overcome the shortcomings of low-dimensional nanowires.However,typical strategies for constructing these superstructures are restricted to complicated and harsh synthetic conditions,not to mention unique 3D structures with advanced properties beyond common superstructures.Herein,we report an unusual network ofα-MnO_(2)nanowires with structure-induced hydrophilicity and conductivity.In the network,the nanowires are interconnected from all directions by nodes,and the 3D network structure is formed from the endless connection of nodes in a node-by-node way.The unique network structure brings about high hydrophilicity and conductivity,both of which are positive factors for an efficient electrocatalyst.Accordingly,the α-MnO_(2) network was tested for electrocatalytic water oxidation and showed significantly enhanced activity compared with isolatedα-MnO_(2)nanowires and 3Dα-MnO_(2)microspheres.This study not only provides a synthetic route toward an advanced network structure but also a new idea for the design of materials for electrochemistry with both efficient mass diffusion and charge transfer.
基金Project(21905232) supported by the National Natural Science Foundation of China。
文摘Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OER). In this work, triangular Cu@CuO nanorods on Cu nanosheets were fabricated by a novel in-situ oxidation approach using Cu nanosheets as self-template and conductive nano-substrate in an aqueous solution of NaOH/H2O2, and then by lowtemperature phosphorization treatments. The experimental results show that the phosphating temperature has a significant effect on the morphology, composition and number of active sites of Cu@Cu_(3)P nanorods. The Cu@Cu_(3)P-280 electrode exhibits a good HER catalytic activity of achieving a current density of 10 mA/cm^(2) at 252 mV in acid electrolyte. After catalysis for 14 h, the current density can still reach 72% of the initial value. Moreover, the Cu@Cu_(3)P-280 electrode also shows an excellent OER catalytic activity in basic electrolyte, reaching a current density of 10 mA/cm^(2) at the overpotential value of 200 mV. After catalysis for 12 h, the current density remained more than 93% of the initial value. This work provides a theoretical basis for the directional design and preparation of sustainable, low-cost, bifunctional electrocatalytic materials.
文摘The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.
文摘Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic oxygen evolution reaction(OER)is still shortage.Herein,we report remarkable promotion of OER performance on the NiFe‐based nanocomposite electrocatalyst via the synergy of multiple carbon‐based interface engineering.Specifically,carbon nanotubes were in situ grown on carbon fiber paper to improve the interface between CFP and NiFeO_(x)H_(y),and graphite carbon nanoparticles were in situ loaded and partly doped into the NiFeO_(x)H_(y) to modify the intergranular interface charge transfer and electronic structure of NiFeO_(x)H_(y).Consequently,the as‐obtained NiFeO_(x)H_(y)‐C/CNTs/CFP catalyst exhibited significantly enhanced electrocatalytic OER activity with an overpotential of 202 mV at 10 mA cm^(-2) in 1 mol L^(-1) KOH.Our work not only extends application of carbon materials but also provides an alternative strategy to develop highly efficient electrocatalysts.
文摘Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increasing attention as active OER catalysts due to their excellent physical and chemical characters,and massive efforts have been devoted to improving the phosphide and sulfide‐based materials with better activity and stability in recent years.In this review,the recent progress on phosphide and sulfide‐based OER electrocatalysts in terms of chemical properties,synthetic methodologies,catalytic performances evaluation and improvement strategy is reviewed.The most accepted reaction pathways as well as the thermodynamics and electrochemistry of the OER are firstly introduced in brief,followed by a summary of the recent research and optimization strategy of phosphide and sulfide‐based OER electrocatalysts.Finally,some mechanistic studies of the active phase of phosphide and sulfide‐based compounds are discussed to give insight into the nature of active catalytic sites.It is expected to indicate guidance for further improving the performances of phosphide and sulfide‐based OER electrocatalysts.
文摘Metal‐organic frameworks(MOFs)are a series of highly porous crystalline materials,which are built from inorganic metal nodes and organic linkers through coordination bonds.Their unique porous structural features(such as high porosity,high surface areas,and highly ordered nanoporous structures)and designable structures and compositions have facilitated their use in gas capture,separation,catalysis,and energy storage and conversion.Recently,the design and synthesis of pure MOFs and their derivatives have opened new routes to develop highly efficient electrocatalysts toward oxygen reduction reactions(ORR)and oxygen evolution reactions(OER),which are the core electrode reactions in many energy storage and conversion techniques,such as metal‐air batteries and fuel cells.This review first discusses recent progress in the synthesis and the electrocatalytic applications of pure MOF‐based electrocatalysts toward ORR or OER,including pure MOFs,MOFs decorated with active species,and MOFs incorporated with conductive materials.The following section focuses on the advancements of the design and preparation of various MOF‐derived materials-such as inorganic nano‐(or micro‐)structures/porous carbon composites,pure porous carbons,pure inorganic nano‐(or micro‐)structured materials,and single‐atom electrocatalysts-and their applications in oxygen electrocatalysis.Finally,we present a conclusion and an outlook for some general design strategies and future research directions of MOF‐based oxygen electrocatalysts.