Lin Li, He Xiaoyang, Zhang Xia-Guang, Ma Wenchao, Zhang Biao, Wei Diye, Xie Shunji, Zhang Qinghong, Yi Xiaodong, Wang Ye
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, P. R. China.
Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, Henan, P. R. China.
Angew Chem Int Ed Engl. 2023 Jan 16;62(3):e202214959. doi: 10.1002/anie.202214959. Epub 2022 Dec 7.
The renewable-electricity-driven CO reduction to formic acid would contribute to establishing a carbon-neutral society. The current catalyst suffers from limited activity and stability under high selectivity and the ambiguous nature of active sites. Herein, we report a powerful Bi S -derived catalyst that demonstrates a current density of 2.0 A cm with a formate Faradaic efficiency of 93 % at -0.95 V versus the reversible hydrogen electrode. The energy conversion efficiency and single-pass yield of formate reach 80 % and 67 %, respectively, and the durability reaches 100 h at an industrial-relevant current density. Pure formic acid with a concentration of 3.5 mol L has been produced continuously. Our operando spectroscopic and theoretical studies reveal the dynamic evolution of the catalyst into a nanocomposite composed of Bi clusters and Bi O CO nanosheets and the pivotal role of Bi -Bi O CO interface in CO activation and conversion.
可再生电力驱动的一氧化碳还原制甲酸将有助于建立一个碳中和社会。目前的催化剂在高选择性下活性和稳定性有限，且活性位点的性质不明确。在此，我们报道了一种强大的铋基衍生催化剂，在相对于可逆氢电极-0.95 V时，其电流密度为2.0 A cm，甲酸盐法拉第效率为93%。甲酸盐的能量转换效率和单程产率分别达到80%和67%，在与工业相关的电流密度下耐久性达到100 h。已连续生产出浓度为3.5 mol L的纯甲酸。我们的原位光谱和理论研究揭示了催化剂动态演变成由铋簇和BiOCO纳米片组成的纳米复合材料，以及Bi-BiOCO界面在CO活化和转化中的关键作用。
