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Enhanced electrochemical CO2 reduction to ethylene over CuO by synergistically tuning oxygen vacancies and metal doping
Cell Reports Physical Science ( IF 8.9 ) Pub Date : 2021-02-24 , DOI: 10.1016/j.xcrp.2021.100356
Yiqiang Jiang , Changhyeok Choi , Song Hong , Senlin Chu , Tai-Sing Wu , Yun-Liang Soo , Leiduan Hao , Yousung Jung , Zhenyu Sun

Electrochemical CO2 reduction to multi-carbon fuels and chemicals is intriguing but remains a challenge. Here, we report that a combination of Sn doping and creation of oxygen vacancies (VO) can synergistically boost CO2 reduction to C2H4 over CuO nanosheets with an onset potential of −0.7 V (versus reversible hydrogen electrode). The activity and selectivity of CuO can be easily tuned by manipulation of Sn dopant and VO contents. The Faradaic efficiency toward C2H4 formation over Sn-doped CuO(VO) approaches 48.5% ± 1.2%, which maintains stability over 24 h at a mild overpotential, in contrast to a maximum of 26.8% ± 2.2% over pristine CuO. The Sn-doped CuO(VO) catalyst presents an approximately 2.3-fold improvement in C2H4 current compared to undoped CuO at similar overpotentials. Theoretical calculations further show that doping of Vo-enriched CuO surface by Sn lowers the dimerization energy of adsorbed CO intermediate, thereby promoting C–C coupling to yield C2H4.



中文翻译:

通过协同调节氧空位和金属掺杂,将电化学CO 2还原成比CuO还原成乙烯的乙烯

用电化学方法将CO 2还原为多碳燃料和化学物质虽然很吸引人,但仍然是一个挑战。在这里,我们报道,Sn掺杂和氧空位(V O)的组合可以协同将Cu 2纳米片上的CO 2还原效率提高到C 2 H 4,起始电位为-0.7 V(相对于可逆氢电极)。通过控制Sn掺杂剂和V O的含量,可以轻松地调节CuO的活性和选择性。Sn掺杂CuO(V O)对C 2 H 4形成的法拉第效率)接近48.5%±1.2%,在温和的超电势下可在24小时内保持稳定性,相比之下,原始CuO的最大值为26.8%±2.2%。与未掺杂的CuO在相似的超电势下相比,掺Sn的CuO(V O)催化剂的C 2 H 4电流提高了约2.3倍。理论计算进一步表明,用Sn掺杂富Vo的CuO表面会降低吸附的CO中间体的二聚能,从而促进C–C偶联生成C 2 H 4

更新日期:2021-03-24
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