Nanosized Pt catalysts are the catalyst-of-choice for proton exchange membrane fuel cell(PEMFC)anode,but are limited by their extreme sensitivity to CO in parts per million(ppm)level,thereby making the use of ultrapur...Nanosized Pt catalysts are the catalyst-of-choice for proton exchange membrane fuel cell(PEMFC)anode,but are limited by their extreme sensitivity to CO in parts per million(ppm)level,thereby making the use of ultrapure H_(2)a prerequisite to ensure acceptable performance.Herein,we confront the CO poisoning issue by bringing the Ir/Rh single atom sites to synergistically working with their metallic counterparts.In presence of 1000 ppm CO,the catalyst represents not only undisturbed H_(2)oxidation reaction(HOR)catalytic behavior in electrochemical cell,but also unparalleled peak power density at 643 mW cm^(-2)in single cell,27-fold in mass activity of the best PtRu/C catalysts available.Pre-poisoning experiments and surface-enhanced Raman scattering spectroscopy(SERS)and calculation results in combine suggest the presence of adjacent Ir/Rh single atom sites(SASs)to the nanoparticles(NPs)as the origin for this prominent catalytic behavior.The single sites not only exhibit superb CO oxidation performance by themselves,but can also scavenge the CO adsorbed on approximated NPs via supplying reactive OH*species.We open up a new route here to conquer the formidable CO poisoning issue through single atom and nanoparticle synergistic catalysis,and pave the way towards a more robust PEMFC future.展开更多
基金National Key R&D Program of China(2020YFB1506800)the National Natural Science Foundation of China(21633008,U1601211,21733004)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21090400)the Jilin Province Science and Technology Development Program(20190201300JC,20170520150JH,20200201001JC)Dalian National Laboratory for Clean Energy(DNL),CAS,the Research Innovation Fund(grant DNL202010)for financial supports。
基金supported by the National Key Research and Development Program of China(2022YFB4004100)the National Natural Science Foundation of China(U22A20396 and 22209168)+1 种基金the Natural Science Foundation of Anhui Province(2208085UD04)China Postdoctoral Science Foundation(2023M743375)。
文摘Nanosized Pt catalysts are the catalyst-of-choice for proton exchange membrane fuel cell(PEMFC)anode,but are limited by their extreme sensitivity to CO in parts per million(ppm)level,thereby making the use of ultrapure H_(2)a prerequisite to ensure acceptable performance.Herein,we confront the CO poisoning issue by bringing the Ir/Rh single atom sites to synergistically working with their metallic counterparts.In presence of 1000 ppm CO,the catalyst represents not only undisturbed H_(2)oxidation reaction(HOR)catalytic behavior in electrochemical cell,but also unparalleled peak power density at 643 mW cm^(-2)in single cell,27-fold in mass activity of the best PtRu/C catalysts available.Pre-poisoning experiments and surface-enhanced Raman scattering spectroscopy(SERS)and calculation results in combine suggest the presence of adjacent Ir/Rh single atom sites(SASs)to the nanoparticles(NPs)as the origin for this prominent catalytic behavior.The single sites not only exhibit superb CO oxidation performance by themselves,but can also scavenge the CO adsorbed on approximated NPs via supplying reactive OH*species.We open up a new route here to conquer the formidable CO poisoning issue through single atom and nanoparticle synergistic catalysis,and pave the way towards a more robust PEMFC future.
基金supported by the National Key Research and Development Program of China (2017YFB0102900)the National Natural Science Foundation of China (21875243, 21633008, 21673221, and U1601211)+3 种基金Jilin Provincial Science and Technology Development Program (20200201001JC, 20190201270JC, and 20180101030JC)supported by the High Performance Computing Center of Jilin University and Jilin ProvinceNetwork and Computing Center of Changchun Institute of Applied Chemistry, Chinese Academy of Sciencessupported by Linglu Instruments (Shanghai) Co., Ltd.