Fe3Mo3C has been prepared and its activity for ammonia synthesis was evaluated.As had been observed previously for Co3Mo3C,it was found to be inactive at 400℃.At 500℃activity developed and this can be related to the...Fe3Mo3C has been prepared and its activity for ammonia synthesis was evaluated.As had been observed previously for Co3Mo3C,it was found to be inactive at 400℃.At 500℃activity developed and this can be related to the substitution of lattice carbon by nitrogen.Application of a simple topotactic route to prepare Ni2Mo3C from Ni2Mo3N proved unsuccessful,with the resultant carbonitride formed under optimal synthesis conditions being active for ammonia synthesis at 400℃.展开更多
表面组分调控及建立多功能活性位点是提高Pt基催化剂性能的有效途径.通过将Cu可控地锚定在纳米结构PtNi表面(Cu/PtNi)可以精确控制Pt基催化剂表面元素的化学计量比,其中亲氧的非贵金属Ni能加速水的解离,Pt由于具有适中的H吸附能,可有效...表面组分调控及建立多功能活性位点是提高Pt基催化剂性能的有效途径.通过将Cu可控地锚定在纳米结构PtNi表面(Cu/PtNi)可以精确控制Pt基催化剂表面元素的化学计量比,其中亲氧的非贵金属Ni能加速水的解离,Pt由于具有适中的H吸附能,可有效地将游离态的H转换成氢气,Cu由于具有正的H吸附吉布斯自由能(ΔG_(H*)),有助于H_(2)的脱附.其中具有最优组分比例的Cu/PtNi电催化剂在海水中表现出优异的电化学析氢活性和稳定性,在碱性海水中,10 mA cm^(-2)下的过电位为23 mV(在70 mV过电位下,其质量活性是商用Pt/C的5倍).同时,密度泛函理论结果进一步验证了在碱性海水中Pt,Ni和Cu多功能金属活性位点可提高HER的H_(2)O解离、H*吸附和H_(2)脱附的过程.展开更多
文摘Fe3Mo3C has been prepared and its activity for ammonia synthesis was evaluated.As had been observed previously for Co3Mo3C,it was found to be inactive at 400℃.At 500℃activity developed and this can be related to the substitution of lattice carbon by nitrogen.Application of a simple topotactic route to prepare Ni2Mo3C from Ni2Mo3N proved unsuccessful,with the resultant carbonitride formed under optimal synthesis conditions being active for ammonia synthesis at 400℃.
基金supported by the National Key Research and Development Program of China(2022YFB3805600,2022YFB3805604,and 2022YFB3806800)the National Natural Science Foundation of China(22293020)+7 种基金the National 111 project(B20002)the Program Fund of Non-Metallic Excellence and Innovation Center for Building Materials(2023TDA1-1)the Program for Changjiang Scholars and Innovative Research Team in University(PCSIRT)(IRT_15R52)Guangdong Basic and Applied Basic Research Foundation(2022A1515010137,2022A1515010504,and 2021A1515111131)Shenzhen Science and Technology Program(GJHZ20210705143204014,JCYJ20210324142010029,and KCXFZ20211020170006010)Hubei Province Key Research and Development Program(2023BAB101)the Fundamental Research Funds for the Central Universities(WUT:2023IVA095 and 2023IV030h)Royal Society for a University Research Fellowship(UF150104,URFR211007)。
文摘表面组分调控及建立多功能活性位点是提高Pt基催化剂性能的有效途径.通过将Cu可控地锚定在纳米结构PtNi表面(Cu/PtNi)可以精确控制Pt基催化剂表面元素的化学计量比,其中亲氧的非贵金属Ni能加速水的解离,Pt由于具有适中的H吸附能,可有效地将游离态的H转换成氢气,Cu由于具有正的H吸附吉布斯自由能(ΔG_(H*)),有助于H_(2)的脱附.其中具有最优组分比例的Cu/PtNi电催化剂在海水中表现出优异的电化学析氢活性和稳定性,在碱性海水中,10 mA cm^(-2)下的过电位为23 mV(在70 mV过电位下,其质量活性是商用Pt/C的5倍).同时,密度泛函理论结果进一步验证了在碱性海水中Pt,Ni和Cu多功能金属活性位点可提高HER的H_(2)O解离、H*吸附和H_(2)脱附的过程.
