Heterogeneous Single-Atom Catalyst for Visible-Light-Driven High-Turnover CO2 Reduction: The Role of Electron Transfer
Heterogeneous Single-Atom Catalyst for Visible-Light-Driven High-Turnover CO2 Reduction: The Role of Electron Transfer
复制标题
用于可见光驱动高转化二氧化碳还原的多相单原子催化剂：电子转移的作用
DOI：
10.1002/adma.201704624
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发表时间：
2018-03-27
影响因子：
29.4
通讯作者：
Xiong, Yujie
中科院分区：
文献类型：
--
作者：
Gao, Chao;Chen, Shuangming;Xiong, Yujie
可见光驱动的二氧化碳转化为化学燃料是解决能源和环境挑战的一个有趣的方法。原则上，结合均相光催化剂和非均相光催化剂的优点，可以优化光收集和催化反应；然而，光吸收剂和催化位点之间的电荷转移效率往往太低，限制了整体光催化性能。在这篇通讯中，报道了在部分氧化的石墨烯纳米片上配位的单原子Co位点可以作为CO2转化的高活性和耐用的非均相催化剂，其中石墨烯桥接均匀的光吸收剂和光激发电子的有效转移的单原子催化位点。结果，CO生成的周转率达到678的高值，周转率为3.77 min(-1)，前所未有，优于目前的多相光催化剂。这项工作从单原子催化的角度为光催化CO2转化的催化位点设计提供了新的见解，并强调了电荷动力学在弥合多相和均相光催化剂之间的差距方面的作用。
Visible-light-driven conversion of CO2 into chemical fuels is an intriguing approach to address the energy and environmental challenges. In principle, light harvesting and catalytic reactions can be both optimized by combining the merits of homogeneous and heterogeneous photocatalysts; however, the efficiency of charge transfer between light absorbers and catalytic sites is often too low to limit the overall photocatalytic performance. In this communication, it is reported that the single-atom Co sites coordinated on the partially oxidized graphene nanosheets can serve as a highly active and durable heterogeneous catalyst for CO2 conversion, wherein the graphene bridges homogeneous light absorbers with single-atom catalytic sites for the efficient transfer of photoexcited electrons. As a result, the turnover number for CO production reaches a high value of 678 with an unprecedented turnover frequency of 3.77 min(-1), superior to those obtained with the state-of-theart heterogeneous photocatalysts. This work provides fresh insights into the design of catalytic sites toward photocatalytic CO2 conversion from the angle of single-atom catalysis and highlights the role of charge kinetics in bridging the gap between heterogeneous and homogeneous photocatalysts.