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Tuning Oxygen Vacancies of Oxides to Promote Electrocatalytic Reduction of Carbon Dioxide
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-01-23 , DOI: 10.1021/acsenergylett.9b02749
Lulu Li 1 , Zhi-Jian Zhao 1 , Congling Hu 1 , Piaoping Yang 1 , Xintong Yuan 1 , Yanan Wang 1 , Lei Zhang 1 , Lyudmila Moskaleva 2, 3 , Jinlong Gong 1
Affiliation  

Tin oxide (SnOx) has emerged as a promising metal oxide catalyst for the CO2 reduction reaction (CO2RR) into value-added chemicals such as formic acid/formate. However, the improvement of SnOx catalytic performance is hindered by its complex surface structures and limited knowledge about the nature of the active sites. This Letter describes the critical role of oxygen vacancies (Ov) in partially reduced SnO2(110) for CO2RR selectivity by combined theoretical and experimental studies. The SnOx with moderate content of Ov is the most active surface and can suppress the undesirable hydrogen evolution reaction simultaneously. This is also confirmed by the electrochemical experiments that also demonstrate that the selectivity of HCOOH changes with varied content of Ov. Further electronic structure analysis reveals that the bond strength and charge transfer between HCOO* and the active site can be regulated by varying the content of Ov, so that the adsorption strength of HCOO* can be tuned.

中文翻译:

调节氧化物的氧空位以促进二氧化碳的电催化还原

氧化锡(SnO x)已成为有前途的金属氧化物催化剂,可用于将CO 2还原反应(CO 2 RR)转化为高附加值的化学品,例如甲酸/甲酸酯。但是,SnO x催化性能的提高由于其复杂的表面结构和对活性位点性质的了解有限而受到阻碍。这封信通过理论和实验研究相结合,描述了氧空位(O v)在部分还原的SnO 2(110)中对CO 2 RR选择性的关键作用。O v含量适中的SnO x是最活跃的表面,可以同时抑制不良的氢释放反应。电化学实验也证实了这一点,电化学实验还证明了HCOOH的选择性随O v含量的变化而变化。进一步的电子结构分析表明,可以通过改变O v的含量来调节HCOO *与活性位之间的键强度和电荷转移,从而可以调节HCOO *的吸附强度。
更新日期:2020-01-24
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