Ji Shufang, Qu Yang, Wang Tao, Chen Yuanjun, Wang Guofeng, Li Xue, Dong Juncai, Chen QiuYu, Zhang Wanying, Zhang Zedong, Liang Shiyou, Yu Rong, Wang Yu, Wang Dingsheng, Li Yadong
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
Key Laboratory of Functional Inorganic Materials Chemistry (Heilongjiang University), Ministry of Education, School of Chemistry and Materials Science, International Joint Research Center for Catalytic Technology, Harbin, 150080, P. R. China.
Angew Chem Int Ed Engl. 2020 Jun 22;59(26):10651-10657. doi: 10.1002/anie.202003623. Epub 2020 Apr 15.
The solar-driven photocatalytic reduction of CO (CO RR) into chemical fuels is a promising route to enrich energy supplies and mitigate CO emissions. However, low catalytic efficiency and poor selectivity, especially in a pure-water system, hinder the development of photocatalytic CO RR owing to the lack of effective catalysts. Herein, we report a novel atom-confinement and coordination (ACC) strategy to achieve the synthesis of rare-earth single erbium (Er) atoms supported on carbon nitride nanotubes (Er /CN-NT) with a tunable dispersion density of single atoms. Er /CN-NT is a highly efficient and robust photocatalyst that exhibits outstanding CO RR performance in a pure-water system. Experimental results and density functional theory calculations reveal the crucial role of single Er atoms in promoting photocatalytic CO RR.
太阳能驱动的光催化将CO还原为化学燃料是丰富能源供应和减少CO排放的一条有前景的途径。然而，由于缺乏有效的催化剂，低催化效率和差的选择性，尤其是在纯水体系中，阻碍了光催化CO还原反应的发展。在此，我们报道了一种新颖的原子限域与配位（ACC）策略，以实现合成负载在氮化碳纳米管上的具有可调单原子分散密度的稀土单铒（Er）原子（Er/CN-NT）。Er/CN-NT是一种高效且稳定的光催化剂，在纯水体系中表现出优异的CO还原反应性能。实验结果和密度泛函理论计算揭示了单Er原子在促进光催化CO还原反应中的关键作用。
