Chen Shaohua, Zhu Chenyuan, Gu Haoyang, Wang Li, Qi Jiajie, Zhong Lixiang, Zhang Zhibin, Yang Chunlei, Shi Guoshuai, Zhao Siwen, Li Shuzhou, Liu Kaihui, Zhang Liming
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China.
Nano Lett. 2021 May 26;21(10):4469-4476. doi: 10.1021/acs.nanolett.1c01258. Epub 2021 May 12.
The electrochemical conversion of CO to valuable fuels is a plausible solution to meet the soaring need for renewable energy sources. However, the practical application of this process is limited by its poor selectivity due to scaling relations. Here we introduce the rational design of the monolayer hexagonal boron nitride/copper (h-BN/Cu) interface to circumvent scaling relations and improve the electrosynthesis of CH. This catalyst possesses a selectivity of >60% toward CH with a production rate of 15 μmol·cm·h at -1.00 V vs RHE, along with a much smaller decaying production rate than that of pristine Cu. Both experimental and theoretical calculations disclosed that h-BN/Cu interfacial perimeters provide specific chelating sites to immobilize the intermediates, which accelerates the conversion of *CO to *CHO. Our work reports a novel Cu catalyst engineering strategy and demonstrates the prospect of monolayer h-BN contributing to the design of heterostructured CO reduction electrocatalysts for sustainable energy conversion.
将一氧化碳电化学转化为有价值的燃料是满足对可再生能源不断飙升需求的一个可行解决方案。然而，由于标度关系，该过程的实际应用受到其选择性差的限制。在此，我们介绍了单层六方氮化硼/铜（h-BN/Cu）界面的合理设计，以规避标度关系并改善CH的电合成。这种催化剂在相对于可逆氢电极（RHE）为-1.00 V时，对CH的选择性大于60%，产率为15 μmol·cm⁻²·h，并且其产率衰减速率比原始铜小得多。实验和理论计算均表明，h-BN/Cu界面周边提供了特定的螯合位点来固定中间体，这加速了CO向CHO的转化。我们的工作报道了一种新型的铜催化剂工程策略，并展示了单层h-BN在设计用于可持续能源转化的异质结构CO还原电催化剂方面的前景。
