Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, Henan, 450001, P. R. China.
Chemistry. 2023 Jun 7;29(32):e202300522. doi: 10.1002/chem.202300522. Epub 2023 Apr 24.
The electroreduction of carbon dioxide (CO ) is a sustainable method for generating valuable chemicals; however, avoiding unwanted hydrogen (H ) production during the electrolysis is a major challenge. Coproduction of carbon monoxide (CO) and H to produce syngas is an effective strategy for solving this problem, and syngas with a desired CO/H ratio can be employed to produce methanol or other valuable chemicals. Herein, a series of palladium-bismuth (Pd-Bi) bimetallic nanochains with different Pd/Bi atomic ratios were prepared and used in the electroreduction of CO to syngas in ionic liquid-based electrolytes. The ratio of CO/H in syngas was regulated in a wide range from 1 : 7 to 9 : 1 by controlling the applied potentials, Pd/Bi atomic ratios and composition of the electrolytes. In particular, the current density reached 19.3 mA cm on Pd Bi bimetallic nanochains at an applied potential of -2.3 V versus Ag/Ag when the CO/H ratio was approximately 1 : 1. Moreover, the maximum CO Faradaic efficiency was 87.7 % for these electrocatalysts at an applied potential of -2.0 V versus Ag/Ag . The synergistic effect of Pd and Bi in the ionic liquid-based electrolyte was the primary reason for the distinct electrocatalytic efficiency of the Pd Bi bimetallic nanochains. The incorporation of moderate amounts of Bi into the Pd lattice resulted in a stronger CO adsorption capacity, more active sites and faster electron transfer rate, which are conducive to improving the electrocatalytic activity.
二氧化碳(CO )的电化学还原是一种生成有价值化学品的可持续方法;然而,避免电解过程中不必要的氢气(H )生成是一个主要挑战。一氧化碳(CO)和 H 的共生产以生成合成气是解决此问题的有效策略,并且可以使用具有所需 CO/H 比的合成气来生产甲醇或其他有价值的化学品。在此,制备了一系列具有不同 Pd/Bi 原子比的钯铋(Pd-Bi)双金属纳米链,并将其用于在离子液体基电解质中 CO 电化学还原为合成气。通过控制施加的电势、Pd/Bi 原子比和电解质的组成,可以在很宽的范围内调节合成气中 CO/H 的比例,从 1:7 到 9:1。特别是,当 CO/H 比约为 1:1 时,在施加的电势为-2.3 V 相对于 Ag/Ag 的 Pd Bi 双金属纳米链上,电流密度达到 19.3 mA cm 。此外,在施加的电势为-2.0 V 相对于 Ag/Ag 时,这些电催化剂的 CO 法拉第效率最高可达 87.7%。Pd 和 Bi 在离子液体基电解质中的协同作用是 Pd Bi 双金属纳米链具有独特电催化效率的主要原因。适量的 Bi 掺入到 Pd 晶格中导致 CO 吸附能力增强、活性位增加和电子转移速率加快,这有利于提高电催化活性。