Liu Li, He Yingchun, Li Qing, Cao Changsheng, Huang Minghong, Ma Dong-Dong, Wu Xin-Tao, Zhu Qi-Long
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou China.
University of Chinese Academy of Sciences Beijing China.
Exploration (Beijing). 2023 Dec 21;4(3):20230043. doi: 10.1002/EXP.20230043. eCollection 2024 Jun.
The coupling electrosynthesis involving CO upgrade conversion is of great significance for the sustainable development of the environment and energy but is challenging. Herein, we exquisitely constructed the self-supported bimetallic array superstructures from the Cu(OH) array architecture precursor, which can enable high-performance coupling electrosynthesis of formate and adipate at the anode and the cathode, respectively. Concretely, the faradaic efficiencies (FEs) of CO-to-formate and cyclohexanone-to-adipate conversion simultaneously exceed 90% at both electrodes with excellent stabilities. Such high-performance coupling electrosynthesis is highly correlated with the porous nanosheet array superstructure of CuBi alloy as the cathode and the nanosheet-on-nanowire array superstructure of CuNi hydroxide as the anode. Moreover, compared to the conventional electrolysis process, the cell voltage is substantially reduced while maintaining the electrocatalytic performance for coupling electrosynthesis in the two-electrode electrolyzer with the maximal FE and FE up to 94.2% and 93.1%, respectively. The experimental results further demonstrate that the bimetal composition modulates the local electronic structures, promoting the reactions toward the target products. Prospectively, our work proposes an instructive strategy for constructing adaptive self-supported superstructures to achieve efficient coupling electrosynthesis.
涉及一氧化碳升级转化的耦合电合成对环境与能源的可持续发展具有重大意义,但极具挑战性。在此,我们巧妙地由氢氧化铜阵列结构前驱体构建了自支撑双金属阵列超结构,其能够分别在阳极和阴极实现高效的甲酸和己二酸耦合电合成。具体而言,在两个电极上,一氧化碳到甲酸以及环己酮到己二酸转化的法拉第效率(FEs)同时超过90%,且具有出色的稳定性。这种高性能耦合电合成与作为阴极的铜铋合金多孔纳米片阵列超结构以及作为阳极的氢氧化铜镍纳米线阵列上的纳米片超结构高度相关。此外,与传统电解过程相比,在双电极电解槽中,在保持耦合电合成电催化性能的同时,电池电压大幅降低,最大法拉第效率分别高达94.2%和93.1%。实验结果进一步表明,双金属组成调节了局部电子结构,促进了向目标产物的反应。前瞻性地看,我们的工作为构建适应性自支撑超结构以实现高效耦合电合成提出了一种指导性策略。