Huang Hui-Zi, Liu Di, Chen Li-Wei, Zhu Zhejiaji, Li Jiani, Yu Zi-Long, Su Xin, Jing Xiaoting, Wu Si-Qian, Tian Wenjing, Yin An-Xiang
Ministry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Advanced Technology Research Institute (Jinan), School of Chemistry and Chemical Engineering, Beijing Institute of Technology Beijing 100081 (P. R. China).
Chem Asian J. 2023 May 2;18(9):e202300110. doi: 10.1002/asia.202300110. Epub 2023 Apr 5.
CO reduction reactions (CO RR) powered by renewable electricity can directly convert CO to hydrocarbons and fix the sustainable but intermittent energy (e. g., sunlight, wind, etc.) in stable and portable chemical fuels. Advanced catalysts boosting CO RR with high activity, selectivity, and durability at low overpotentials are of great importance but still elusive. Here, we report that the ultrathin Pd-Ag dendritic nanoplates (PdAg DNPs) exhibited boosted activity, selectivity, and stability for producing formate from CO at a very low overpotential in aqueous solutions under ambient conditions. As a result, the PdAg DNPs exhibited a Faradaic efficiency (FE) for formate of 91% and a cathodic energy efficiency (EE) of ∼90% at the potential of -0.2 V versus reversible hydrogen electrode (vs. RHE), showing significantly enhanced durability as compared with pure Pd catalysts. Our strategy represents a rational catalyst design by engineering the surface geometrical and electronic structures of metal nanocrystals and may find more applicability in future electrocatalysis.
由可再生电力驱动的一氧化碳还原反应(CO RR)可直接将CO转化为碳氢化合物,并将可持续但间歇性的能源(如阳光、风能等)固定在稳定且便于携带的化学燃料中。开发在低过电位下具有高活性、选择性和耐久性的先进CO RR催化剂至关重要,但仍难以实现。在此,我们报道了超薄钯银树枝状纳米片(PdAg DNP)在环境条件下的水溶液中,在极低过电位下对由CO生成甲酸盐表现出增强的活性、选择性和稳定性。结果,在相对于可逆氢电极(vs. RHE)为-0.2 V的电位下,PdAg DNP对甲酸盐的法拉第效率(FE)为91%,阴极能量效率(EE)约为90%,与纯钯催化剂相比,其耐久性显著提高。我们的策略是通过设计金属纳米晶体的表面几何结构和电子结构进行合理的催化剂设计,可能在未来的电催化中具有更多适用性。