直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO...直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO毒化,降低了催化剂的稳定性和寿命,这些因素都抑制了催化剂的实际应用.本文中,我们报道了一种用于乙醇氧化反应的具有不同Rh含量的超细三金属PtNiRh纳米线,Pt_(6)Ni_(2)Rh_(3)/C具有最优的催化活性(1.16 A mg_(Pt^(-1)))、抗CO中毒能力和稳定性.理论计算表明,在双金属PtNi中引入Rh,使得该催化剂具有良好的中间物吸附和C–C键断裂能力,有利于乙醇的完全氧化.展开更多
Heterogeneous single-atom catalysts(SACs)hold the promise of combining high catalytic performance with maximum utilization of often precious metals.We extend the current thermodynamic view of SAC stability in terms of...Heterogeneous single-atom catalysts(SACs)hold the promise of combining high catalytic performance with maximum utilization of often precious metals.We extend the current thermodynamic view of SAC stability in terms of the binding energy(E_(bind))of singlemetal atoms on a support to a kinetic(transport)one by considering the activation barrier for metal atom diffusion.A rapid computational screening approach allows predicting diffusion barriers for metal-support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal(E_(c)).展开更多
开发高效的铂(Pt)基电催化剂对于燃料电池的发展具有极其重要的意义.本文报道了一种氮掺杂纳米碳结构包覆的超低Pt合金集成电催化剂并用于燃料电池氧还原反应.该Pt基催化剂复合材料在0.9 V vs.RHE的电位下展现出3.46 A mg^(-1)_(Pt)质...开发高效的铂(Pt)基电催化剂对于燃料电池的发展具有极其重要的意义.本文报道了一种氮掺杂纳米碳结构包覆的超低Pt合金集成电催化剂并用于燃料电池氧还原反应.该Pt基催化剂复合材料在0.9 V vs.RHE的电位下展现出3.46 A mg^(-1)_(Pt)质量活性,并且在10000圈循环后几乎没有衰减.单电池测试结果表明,其Pt利用率高达10.22 W mg^(-1)_(Pt)阴极,并具有30000圈循环的优异耐久性.实验和理论研究表明,将Co/Ni掺入Pt晶格可产生具有最佳Pt-O结合能的高应变Pt结构,这可显著加快反应动力学.氮掺杂纳米碳结构和活性Pt组分产生的协同催化作用是提高催化活性的主要原因,同时增强的金属-载体相互作用和优化的亲水性能可促进传质过程和水管理.这项工作可为燃料电池及其他领域的低Pt集成电催化剂的设计提供重要见解.展开更多
基金supported by The Netherlands Organization for Scientific Research(NWO)through a Vici grant and Nuffic fundingfunding from the European Union’s Horizon 2020 research and innovation programme under grant No.686086(Partial-PGMs)。
基金financially supported by the National Natural Science Foundation of China (22275102)the Natural Science Foundation of Tianjin (20JCYBJC01330)+1 种基金Haihe Laboratory of Sustainable Chemical Transformationsthe "Young Talent Support Plan" of Xi’an Jiaotong University
基金supported by Hainan Province Science and Technology Special Fund(ZDYF2021GXJS207,ZDYF2020037,and 2020207)the National Natural Science Foundation of China(22109034,22109035,52164028,and 62105083)+2 种基金the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,MRUKF2021029)the specific research fund of the Innovation Platform for Academicians of Hainan Provincethe“Young Talent Support Plan”of Xi’an Jiaotong University。
文摘直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO毒化,降低了催化剂的稳定性和寿命,这些因素都抑制了催化剂的实际应用.本文中,我们报道了一种用于乙醇氧化反应的具有不同Rh含量的超细三金属PtNiRh纳米线,Pt_(6)Ni_(2)Rh_(3)/C具有最优的催化活性(1.16 A mg_(Pt^(-1)))、抗CO中毒能力和稳定性.理论计算表明,在双金属PtNi中引入Rh,使得该催化剂具有良好的中间物吸附和C–C键断裂能力,有利于乙醇的完全氧化.
基金the Natural Science Foundation of Hainan Province(2019RC007)the National Natural Science Foundation of China(21805104,21606050,21905056,21905045,and U1801257)+3 种基金the Natural Science Foundation of Guangdong Province(2018A0303130239,2018A0303130223)Pearl River Science and Technology New Star Project(201806010039)the Start-up Research Foundation of Hainan University(KYQD(ZR)1908)Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province。
基金This work has received funding from the European Union’s Horizon 2020 research and innovation programme under grant No 686086(Partial-PGMs)Y.W.,K.A.,and D.G.V.acknowledge support by the RAPID manufacturing institute,supported by the Department of Energy(DOE)Advanced Manufacturing Office(AMO),award number DE-EE0007888-9.5.
文摘Heterogeneous single-atom catalysts(SACs)hold the promise of combining high catalytic performance with maximum utilization of often precious metals.We extend the current thermodynamic view of SAC stability in terms of the binding energy(E_(bind))of singlemetal atoms on a support to a kinetic(transport)one by considering the activation barrier for metal atom diffusion.A rapid computational screening approach allows predicting diffusion barriers for metal-support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal(E_(c)).
基金the National Natural Science Foundation of China(22075092 and 21805104)the Program for Huazhong University of Science and Technology(HUST)Academic Frontier Youth Team(2018QYTD15)The Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘开发高效的铂(Pt)基电催化剂对于燃料电池的发展具有极其重要的意义.本文报道了一种氮掺杂纳米碳结构包覆的超低Pt合金集成电催化剂并用于燃料电池氧还原反应.该Pt基催化剂复合材料在0.9 V vs.RHE的电位下展现出3.46 A mg^(-1)_(Pt)质量活性,并且在10000圈循环后几乎没有衰减.单电池测试结果表明,其Pt利用率高达10.22 W mg^(-1)_(Pt)阴极,并具有30000圈循环的优异耐久性.实验和理论研究表明,将Co/Ni掺入Pt晶格可产生具有最佳Pt-O结合能的高应变Pt结构,这可显著加快反应动力学.氮掺杂纳米碳结构和活性Pt组分产生的协同催化作用是提高催化活性的主要原因,同时增强的金属-载体相互作用和优化的亲水性能可促进传质过程和水管理.这项工作可为燃料电池及其他领域的低Pt集成电催化剂的设计提供重要见解.
