▌Molecular Bottom-Up Design of Single-Site Copper-Palladium Catalysts for Selective Glycerol Electro-Oxidation
用於選擇性甘油電氧化之銅鈀雙金屬單位點催化劑的分子自下而上設計
S. A. Chala*, E. O. Oseghe, K. Lakshmanan, M. Langer, K. Potemkin, P. Heim, R. Liu, T. R. Studer, M. C. Tsai, K. Cao, C. C. Chang, C. Y. Chang, K. Sowa, E. Ebrahimi, S. Rahali, S. T. Clausing, S. S. Akbari, J. Bansmann, B. J. Hwang* and C. Streb*
https://doi.org/10.1002/aenm.202504456
SEED Member: B. J. Hwang, M. C. Tsai
Major Contributions
1. A molecular bottom-up approach designs a bimetallic Cu-Pd single-site catalyst (SSC) with CuN₄/PdN₄ moieties, achieving 83% Faradaic efficiency for formate and 16% for C3 products in glycerol electrooxidation (GOR) at 1.0 V vs. RHE.
2. Operando spectroscopy and DFT reveal that Pd sites facilitate C-OH adsorption, preventing C-C bond cleavage and catalyst poisoning by CO/CO₃²⁻, while the synergistic CuN₄/PdN₄ coordination governs product selectivity.
3. The catalyst maintains stable performance for 144 h at 50 mA cm⁻², validating the SSC design as a selective and durable strategy for producing value-added formate and C3 chemicals from biomass-derived glycerol.
主要貢獻
1. 以分子自下而上方法設計具有 CuN₄/PdN₄ 配位的雙金屬 Cu-Pd 單位點催化劑,在甘油電氧化(GOR)中於 1.0 V vs. RHE 實現甲酸鹽法拉第效率 83%、C3 產物 16%。
2. 原位光譜與 DFT 揭示 Pd 位點促進 C-OH 吸附,防止 C-C 鍵斷裂與 CO/CO₃²⁻ 催化劑中毒,CuN₄/PdN₄ 協同配位決定產物選擇性。
3. 催化劑在 50 mA cm⁻² 下穩定運行 144 小時,驗證 SSC 設計是從生質衍生甘油生產增值甲酸鹽與 C3 化學品的選擇性持久策略。





