Li Yicheng, Delmo Ernest Pahuyo, Hou Guoyu, Cui Xianglong, Zhao Ming, Tian Zhihong, Zhang Yu, Shao Minhua
School of Mechanical and Power Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology Clear Water Bay, Kowloon, Hong Kong, China.
Angew Chem Int Ed Engl. 2023 Dec 4;62(49):e202313522. doi: 10.1002/anie.202313522. Epub 2023 Oct 31.
Electrochemical carbon dioxide reduction reaction (CO RR) to produce valuable chemicals is a promising pathway to alleviate the energy crisis and global warming issues. However, simultaneously achieving high Faradaic efficiency (FE) and current densities of CO RR in a wide potential range remains as a huge challenge for practical implements. Herein, we demonstrate that incorporating bismuth-based (BH) catalysts with L-histidine, a common amino acid molecule of proteins, is an effective strategy to overcome the inherent trade-off between the activity and selectivity. Benefiting from the significantly enhanced CO adsorption capability and promoted electron-rich nature by L-histidine integrity, the BH catalyst exhibits excellent FE in the unprecedented wide potential windows (>90 % within -0.1--1.8 V and >95 % within -0.2--1.6 V versus reversible hydrogen electrode, RHE). Excellent CO RR performance can still be achieved under the low-concentration CO feeding (e.g., 20 vol.%). Besides, an extremely low onset potential of -0.05 V (close to the theoretical thermodynamic potential of -0.02 V ) was detected by in situ ultraviolet-visible (UV-Vis) measurements, together with stable operation over 50 h with preserved FE of ≈95 % and high partial current density of 326.2 mA cm at -1.0 V .
通过电化学二氧化碳还原反应（CO₂RR）制备有价值的化学品是缓解能源危机和全球变暖问题的一条很有前景的途径。然而，在很宽的电位范围内同时实现高法拉第效率（FE）和CO₂RR电流密度，对于实际应用而言仍然是一个巨大的挑战。在此，我们证明将铋基（BH）催化剂与蛋白质中常见的氨基酸分子L-组氨酸相结合，是克服活性与选择性之间固有权衡的有效策略。得益于L-组氨酸的完整性显著增强了CO吸附能力并促进了富电子性质，BH催化剂在前所未有的宽电位窗口内表现出优异的FE（相对于可逆氢电极，RHE，在-0.1--1.8 V范围内>90%，在-0.2--1.6 V范围内>95%）。在低浓度CO进料（例如20 vol.%）的情况下仍可实现优异的CO₂RR性能。此外，通过原位紫外-可见（UV-Vis）测量检测到极低的起始电位为-0.05 V（接近理论热力学电位-0.02 V），并且在-1.0 V下稳定运行超过50小时，FE保持在≈95%，部分电流密度高达326.2 mA cm² 。
