Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysi...Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysis systems based on cobalt-based monofunctional hydrogen evolution reaction(HER)or oxygen evolution reaction(OER)catalysts have certain shortcomings in terms of resource utilization and universality.In contrast,cobalt-based bifunctional catalysts(CBCs)have attracted much attention in recent years for overall water splitting systems because of their practicality and reduced preparation cost of electrolyzer.This review aims to address the latest development in CBCs for total hydrolysis.The main modification strategies of CBCs are systematically classified in water electrolysis to provide an overview of how to regulate their morphology and electronic configuration.Then,the catalytic performance of CBCs in total-hydrolysis is summarized according to the types of cobalt-based phosphides,sulfides and oxides,and the mechanism of strengthened electrocatalytic ability is emphasized through combining experiments and theoretical calculations.Future efforts are finally suggested to focus on exploring the dynamic conversion of reaction intermediates and building near-industrial CBCs,designing advanced CBC materials through micro-modulation,and addressing commercial applications.展开更多
Reducing the cost and improving the electrocatalytic activity are the key to developing high efficiency electrocatalysts for oxygen evolution reaction(OER).Here,bimetallic NiFe-based metal-organic framework(MOF)was pr...Reducing the cost and improving the electrocatalytic activity are the key to developing high efficiency electrocatalysts for oxygen evolution reaction(OER).Here,bimetallic NiFe-based metal-organic framework(MOF)was prepared by solvothermal method,and then used as precursor to prepare NiFe-based MOF-derived materials by pyrolysis.The effects of different metal ratios and pyrolysis temperatures on the sample structure and OER electrocatalytic performance were investigated and compared.The experimental results showed that when the metal molar ratio was Fe:Ni=1:5 and the pyrolysis temperature was 450℃,the sample(FeNi_(5)-MOF-450)exhibits a composite structure of Ni Fe_(2)O_(4)/FeNi_(3)/C and owns the superior electrocatalytic activity in OER.When the current density is 100 mA·cm^(-2),the overpotential of the sample was 377 mV with Tafel slope of 56.2 mV·dec^(-1),which indicates that FeNi_(5)-MOF-450 exhibits superior electrocatalytic performance than the commercial RuO_(2).Moreover,the long-term stability of FeNi_(5)-MOF-450 further promotes its development in OER.This work demonstrated that the regulatory methods such as component optimization can effectively improve the OER catalytic performance of NiFe-based MOF-derived materials.展开更多
A novel plastic/multi-walled carbon nanotube(MWNTs)-nickel(Ni)-platinum(Pt) electrode(PMNP) is prepared by chemical-reducing Pt onto the surface of Ni film covered plastic/MWNTs(PM) substrate. The MWNTs are ...A novel plastic/multi-walled carbon nanotube(MWNTs)-nickel(Ni)-platinum(Pt) electrode(PMNP) is prepared by chemical-reducing Pt onto the surface of Ni film covered plastic/MWNTs(PM) substrate. The MWNTs are adhered by a piece of commercial double faced adhesive tape on the surface of plastic paper and the Ni film is prepared by a simple electrodeposition method. The morphology and phase structure of the PMNP electrode are characterized by scanning electron microscopy,transmission electron microscope and X-ray diffractometer. The catalytic activity of the PMNP electrode for Na BH4 electrooxidation is investigated by means of cyclic voltammetry and chronoamperometry. The catalyst combines tightly with the plastic paper and exhibits a good stability. MWNTs serve as both conductive material and hydrogen storage material and the Ni film and Pt are employed as electrochemical catalysts. The PMNP electrode exhibits a high electrocatalytic performance and the oxidation current density reaches to 10.76 A/(mg·cm) in 0.1 mol/dm3 Na BH4at0 V,which is much higher than those in the previous reports. The using of waste plastic reduces the discarding of white pollution and consumption of metal resources.展开更多
Noble metal-based intermetallics are promising electrocatalysts for sustainable energy conversion and consumption processes.High-temperature pyrolysis(>500°C)methods are used to control their crystalline order...Noble metal-based intermetallics are promising electrocatalysts for sustainable energy conversion and consumption processes.High-temperature pyrolysis(>500°C)methods are used to control their crystalline orderings,critical to their electrocatalytic activity and durability.However,the high temperature would cause severe aggregation,resulting in a low catalytic active surface area.Significant research efforts have been devoted to addressing this issue.This short review summarizes recent research progress on synthesizing noble metal-based intermetallic electrocatalysts by space-confined pyrolysis.We focus on three strategies:isolation in pores,coverture by shells,and immobilization by salts.The advantages and existing problems of different methods are highlighted.Last,important issues to be addressed in future research are also discussed.We hope that this article will stimulate future research to develop high-performance intermetallic catalysts for practical applications.展开更多
Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread application...Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread applications. Herein, fullerene molecules(i.e., C60and C70) have been successfully introduced into the pore-channels of a Co-porphyrin based MOF through a facile strategy. Thus-obtained hybrid materials present higher electron-transfer ability, enhanced CO_(2)adsorption-enthalpy and CO_(2)electroreduction activity. Notably, the charge transfer resistance(Rct) of C60@MOF-545-Co is almost 5 times lower of than that of MOF-545-Co, as well as 1.5 times increased for the CO_(2)adsorption enthalpy. As expect, the FECO of C60@MOF-545-Co(97.0%) is largely higher than MOF-545-Co(70.2%), C60@MOF-545(19.4%), C60(11.5%)and physical mixture(70.3%) and presented as one of the best CO_(2)electroreduction catalysts reported in H-cell system. The facile strategy would give rise to new insight into the exploration of powerful MOFbased hybrid materials in high-efficiency CO_(2)electroreduction.展开更多
Today,nanocrystals enclosed by high-index facets(HIFs)are attracting widely attentions of researchers due to their tremendous potential in the field of catalysis,especially in electrocatalysis,such as electro-oxidatio...Today,nanocrystals enclosed by high-index facets(HIFs)are attracting widely attentions of researchers due to their tremendous potential in the field of catalysis,especially in electrocatalysis,such as electro-oxidation of small organic molecule(such as formic acid,methanol,and ethanol),oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),as well as the oxygen evolution reaction(OER).However,the practical applications of nanocrystals enclosed by HIFs still face many limitations in preparations of advanced electrocatalysts,including preparation strategy,limited life-time and stability.The development of advanced electrocatalysts enclosed with HIFs is crucial for solving these problems if the large-scale application of them is to be realized.Herein,we firstly detailedly demonstrate the identification methods of nanocrystals enclosed by HIFs,and then preparation strategies are elaborated in detail in this review.Current advanced nanocrystals enclosed by HIFs in electrocatalytic application are also summarized and we present representative achievements to further reveal the relationship of excellent electrocatalytic performance and nanocrystals with HIFs.Finally,we predict the remaining challenges and present our perspectives with regards of design strategies of improving electrocatalytic performance of Ptbased catalysts in the future.展开更多
Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considera...Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considerable research efforts have been devoted to construct advanced fiber materials possessing conductive network(to facilitate efficient electron transport)and large specific surface area(to support massive catalytically active sites)to boost electrocatalysis performance.Herein,we focused on recent advances in fiber-based electrocatalyst with enhanced electrocatalytic activity.Moreover,the synthesis,structure,and properties of fiber materials and their applications in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction are discussed.Finally,the research challenges and future prospects of fiber materials in electrocatalysis applications are proposed.展开更多
基金financially supported by the National Natural Science Foundation of China(51572166,52102070)the Program for Professor of Special Appointment at Shanghai Institutions of Higher Learning(GZ2020012)+4 种基金the Key Research Project of Zhejiang Laboratory(2021PE0AC02)the China Postdoctoral Science Foundation(2021M702073)BAJC R&D Fund Projects(BA23011)Australian Research Council Future Fellowships(FT230100436)the Shanghai Technical Service Center for Advanced Ceramics Structure Design and Precision Manufacturing(20DZ2294000)。
文摘Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysis systems based on cobalt-based monofunctional hydrogen evolution reaction(HER)or oxygen evolution reaction(OER)catalysts have certain shortcomings in terms of resource utilization and universality.In contrast,cobalt-based bifunctional catalysts(CBCs)have attracted much attention in recent years for overall water splitting systems because of their practicality and reduced preparation cost of electrolyzer.This review aims to address the latest development in CBCs for total hydrolysis.The main modification strategies of CBCs are systematically classified in water electrolysis to provide an overview of how to regulate their morphology and electronic configuration.Then,the catalytic performance of CBCs in total-hydrolysis is summarized according to the types of cobalt-based phosphides,sulfides and oxides,and the mechanism of strengthened electrocatalytic ability is emphasized through combining experiments and theoretical calculations.Future efforts are finally suggested to focus on exploring the dynamic conversion of reaction intermediates and building near-industrial CBCs,designing advanced CBC materials through micro-modulation,and addressing commercial applications.
基金supported by the Shandong Natural Science Fund (No.ZR2020KB010)the Fundamental Research Funds for the Central Universities (No.22CX 07010A)。
文摘Reducing the cost and improving the electrocatalytic activity are the key to developing high efficiency electrocatalysts for oxygen evolution reaction(OER).Here,bimetallic NiFe-based metal-organic framework(MOF)was prepared by solvothermal method,and then used as precursor to prepare NiFe-based MOF-derived materials by pyrolysis.The effects of different metal ratios and pyrolysis temperatures on the sample structure and OER electrocatalytic performance were investigated and compared.The experimental results showed that when the metal molar ratio was Fe:Ni=1:5 and the pyrolysis temperature was 450℃,the sample(FeNi_(5)-MOF-450)exhibits a composite structure of Ni Fe_(2)O_(4)/FeNi_(3)/C and owns the superior electrocatalytic activity in OER.When the current density is 100 mA·cm^(-2),the overpotential of the sample was 377 mV with Tafel slope of 56.2 mV·dec^(-1),which indicates that FeNi_(5)-MOF-450 exhibits superior electrocatalytic performance than the commercial RuO_(2).Moreover,the long-term stability of FeNi_(5)-MOF-450 further promotes its development in OER.This work demonstrated that the regulatory methods such as component optimization can effectively improve the OER catalytic performance of NiFe-based MOF-derived materials.
基金supported by the Fundamental Research Funds for the Central Universities (HEUCF201403018)the Heilongjiang Postdoctoral Fund (LBHZ13059)+1 种基金the China Postdoctoral Science Foundation (2014M561332)the National Natural Science Foundation of China (21403044)
文摘A novel plastic/multi-walled carbon nanotube(MWNTs)-nickel(Ni)-platinum(Pt) electrode(PMNP) is prepared by chemical-reducing Pt onto the surface of Ni film covered plastic/MWNTs(PM) substrate. The MWNTs are adhered by a piece of commercial double faced adhesive tape on the surface of plastic paper and the Ni film is prepared by a simple electrodeposition method. The morphology and phase structure of the PMNP electrode are characterized by scanning electron microscopy,transmission electron microscope and X-ray diffractometer. The catalytic activity of the PMNP electrode for Na BH4 electrooxidation is investigated by means of cyclic voltammetry and chronoamperometry. The catalyst combines tightly with the plastic paper and exhibits a good stability. MWNTs serve as both conductive material and hydrogen storage material and the Ni film and Pt are employed as electrochemical catalysts. The PMNP electrode exhibits a high electrocatalytic performance and the oxidation current density reaches to 10.76 A/(mg·cm) in 0.1 mol/dm3 Na BH4at0 V,which is much higher than those in the previous reports. The using of waste plastic reduces the discarding of white pollution and consumption of metal resources.
基金financially supported by the National Key Research and Development Program(2018YFB1502503)the Sichuan Science and Technology Program(2020YJ0299)financial supports from the Australian Research Council under the future fellowship scheme(FT160100107)。
文摘Noble metal-based intermetallics are promising electrocatalysts for sustainable energy conversion and consumption processes.High-temperature pyrolysis(>500°C)methods are used to control their crystalline orderings,critical to their electrocatalytic activity and durability.However,the high temperature would cause severe aggregation,resulting in a low catalytic active surface area.Significant research efforts have been devoted to addressing this issue.This short review summarizes recent research progress on synthesizing noble metal-based intermetallic electrocatalysts by space-confined pyrolysis.We focus on three strategies:isolation in pores,coverture by shells,and immobilization by salts.The advantages and existing problems of different methods are highlighted.Last,important issues to be addressed in future research are also discussed.We hope that this article will stimulate future research to develop high-performance intermetallic catalysts for practical applications.
基金financially supported by the National Natural Science Foundation of China (Nos. 22171139 and 21901122)Natural Science Foundation of Educational Commission of Anhui Province of China (No. KJ2020A0240)+1 种基金the Natural Science Research of Jiangsu Higher Education Institutions of China (No.19KJB150011)Project funded by China Postdoctoral Science Foundation (No. 2019M651873)。
文摘Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread applications. Herein, fullerene molecules(i.e., C60and C70) have been successfully introduced into the pore-channels of a Co-porphyrin based MOF through a facile strategy. Thus-obtained hybrid materials present higher electron-transfer ability, enhanced CO_(2)adsorption-enthalpy and CO_(2)electroreduction activity. Notably, the charge transfer resistance(Rct) of C60@MOF-545-Co is almost 5 times lower of than that of MOF-545-Co, as well as 1.5 times increased for the CO_(2)adsorption enthalpy. As expect, the FECO of C60@MOF-545-Co(97.0%) is largely higher than MOF-545-Co(70.2%), C60@MOF-545(19.4%), C60(11.5%)and physical mixture(70.3%) and presented as one of the best CO_(2)electroreduction catalysts reported in H-cell system. The facile strategy would give rise to new insight into the exploration of powerful MOFbased hybrid materials in high-efficiency CO_(2)electroreduction.
基金financially supported by the National Natural Science Foundation of China(No.22008135)the China Postdoctoral Science Foundation(No.2020M670345)。
文摘Today,nanocrystals enclosed by high-index facets(HIFs)are attracting widely attentions of researchers due to their tremendous potential in the field of catalysis,especially in electrocatalysis,such as electro-oxidation of small organic molecule(such as formic acid,methanol,and ethanol),oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),as well as the oxygen evolution reaction(OER).However,the practical applications of nanocrystals enclosed by HIFs still face many limitations in preparations of advanced electrocatalysts,including preparation strategy,limited life-time and stability.The development of advanced electrocatalysts enclosed with HIFs is crucial for solving these problems if the large-scale application of them is to be realized.Herein,we firstly detailedly demonstrate the identification methods of nanocrystals enclosed by HIFs,and then preparation strategies are elaborated in detail in this review.Current advanced nanocrystals enclosed by HIFs in electrocatalytic application are also summarized and we present representative achievements to further reveal the relationship of excellent electrocatalytic performance and nanocrystals with HIFs.Finally,we predict the remaining challenges and present our perspectives with regards of design strategies of improving electrocatalytic performance of Ptbased catalysts in the future.
基金The funding has been received from Fundamental Research Funds for the Central Universities with Grant no.2232021A-02Shanghai Committee of Science and Technology,China with Grant No.21ZR1480000National Natural Science Foundation of China with Grant Nos.52122312,52172291.
文摘Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considerable research efforts have been devoted to construct advanced fiber materials possessing conductive network(to facilitate efficient electron transport)and large specific surface area(to support massive catalytically active sites)to boost electrocatalysis performance.Herein,we focused on recent advances in fiber-based electrocatalyst with enhanced electrocatalytic activity.Moreover,the synthesis,structure,and properties of fiber materials and their applications in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction are discussed.Finally,the research challenges and future prospects of fiber materials in electrocatalysis applications are proposed.