Energy conversion technologies like fuel cells and metal-air batteries require oxygen reduction reaction(ORR)electrocatalysts with low cost and high catalytic activity.Herein,N-doped carbon spheres(N-CS)with rich micr...Energy conversion technologies like fuel cells and metal-air batteries require oxygen reduction reaction(ORR)electrocatalysts with low cost and high catalytic activity.Herein,N-doped carbon spheres(N-CS)with rich micropore structure have been synthesized by a facile two-step method,which includes the polymerization of pyrrole and formaldehyde and followed by a facile pyrolysis process.During the preparation,zinc chloride(ZnCl2)was utilized as a catalyst to promote polymerization and provide a hypersaline environment.In addition,the morphology,defect content and activity area of the resultant N-CS catalysts could be regulated by controlling the content of ZnCl2.The optimum N-CS-1 catalyst demonstrated much better catalytic activity and durability towards ORR in alkaline conditions than commercial 20 wt%Pt/C catalysts,of which the half-wave potential reached 0.844 V vs.RHE.When applied in the Zn-air batteries as cathode catalysts,N-CS-1 showed a maximum power density of 175 mW cm^(-2) and long-term discharging stability of over 150 h at 10 mA cm^(-2),which outperformed 20 wt%Pt/C.The excellent performance could be due to its ultrahigh specific surface area of 1757 m2 g1 and rich micropore channels structure.Meanwhile,this work provides an efficient method to synthesize an ultrahigh surface porous carbon material,especially for catalyst application.展开更多
Electrocatalytic water splitting(EWS)is a promising route to produce hydrogen in a sustainable and environment-benign manner.To realize the large-scale hydrogen production,it is paramount to develop desirable electroc...Electrocatalytic water splitting(EWS)is a promising route to produce hydrogen in a sustainable and environment-benign manner.To realize the large-scale hydrogen production,it is paramount to develop desirable electrocatalysts with engineered structure,high catalytic activity,facile accessibility,low cost,and good durability.Of late,boride-based materials,especially transition-metal borides(TMBs),are emerging as promising candidates for the EWS process.However,so far,ittle attempt has been made to provide a comprehensive summary on these findings.Herein,this review provides the up-to-date status on upgrading the catalytic performance of TMB-based nanomaterials by regulating the internal and external characteristics.The conventional synthetic techniques are first presented for the preparation of TMB-based catalysts.Afterwards,the advanced strategies are summarized to enhance the catalytic performance of TMBs,including morphology control,component regulation,phase engineering,surface oxidation and hybridization.Then,the design principles of TMB-based electrocatalysts for high-performance EWS are outined.Lastly,the current challenges and future directions in the development of TMB-based materials are proposed.This review article is expected to envisage insights into the TMBs-based water splitting and to provide strategies for design of the next-generation TMB-based electrocatalysts.展开更多
基金financially supported by the National Key R&D Program of China (No. 2018YFB0104000 and No. 2019YFA0210300)National Nature Science Foundation of China (No.21571189 and No.21671200)+3 种基金Natural Science Foundation of Jiangsu Province (BK20200991)Hunan Provincial Science and Technology Plan Project of China (No. 2019GK2033, No. 2017TP1001, CPS2019K06 and No. 2018RS3009)Postdoctoral International Exchange Program Funding of China (No. [2018]115)China Postdoctoral Science Foundation (2019M652802)
文摘Energy conversion technologies like fuel cells and metal-air batteries require oxygen reduction reaction(ORR)electrocatalysts with low cost and high catalytic activity.Herein,N-doped carbon spheres(N-CS)with rich micropore structure have been synthesized by a facile two-step method,which includes the polymerization of pyrrole and formaldehyde and followed by a facile pyrolysis process.During the preparation,zinc chloride(ZnCl2)was utilized as a catalyst to promote polymerization and provide a hypersaline environment.In addition,the morphology,defect content and activity area of the resultant N-CS catalysts could be regulated by controlling the content of ZnCl2.The optimum N-CS-1 catalyst demonstrated much better catalytic activity and durability towards ORR in alkaline conditions than commercial 20 wt%Pt/C catalysts,of which the half-wave potential reached 0.844 V vs.RHE.When applied in the Zn-air batteries as cathode catalysts,N-CS-1 showed a maximum power density of 175 mW cm^(-2) and long-term discharging stability of over 150 h at 10 mA cm^(-2),which outperformed 20 wt%Pt/C.The excellent performance could be due to its ultrahigh specific surface area of 1757 m2 g1 and rich micropore channels structure.Meanwhile,this work provides an efficient method to synthesize an ultrahigh surface porous carbon material,especially for catalyst application.
基金This work is supported by the Australian Research Council(ARC)Future Fellowship(No.FT 160100195)Z.J.C.would like to acknowledge the China Scholarship Council(CSC)for the scholarship support.
文摘Electrocatalytic water splitting(EWS)is a promising route to produce hydrogen in a sustainable and environment-benign manner.To realize the large-scale hydrogen production,it is paramount to develop desirable electrocatalysts with engineered structure,high catalytic activity,facile accessibility,low cost,and good durability.Of late,boride-based materials,especially transition-metal borides(TMBs),are emerging as promising candidates for the EWS process.However,so far,ittle attempt has been made to provide a comprehensive summary on these findings.Herein,this review provides the up-to-date status on upgrading the catalytic performance of TMB-based nanomaterials by regulating the internal and external characteristics.The conventional synthetic techniques are first presented for the preparation of TMB-based catalysts.Afterwards,the advanced strategies are summarized to enhance the catalytic performance of TMBs,including morphology control,component regulation,phase engineering,surface oxidation and hybridization.Then,the design principles of TMB-based electrocatalysts for high-performance EWS are outined.Lastly,the current challenges and future directions in the development of TMB-based materials are proposed.This review article is expected to envisage insights into the TMBs-based water splitting and to provide strategies for design of the next-generation TMB-based electrocatalysts.