Key Laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint Laboratory on New Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
CAS-HKU Joint Laboratory on New Materials & Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong SAR, P. R. China.
Angew Chem Int Ed Engl. 2023 Mar 6;62(11):e202300094. doi: 10.1002/anie.202300094. Epub 2023 Feb 2.
Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H is an ideal solution to address severe plastic pollution. Here, we report the electrooxidation of EG to glycolic acid (GA) with a high Faraday efficiency and selectivity (>85 %) even at an industry-level current density (600 mA cm at 1.15 V vs. RHE) over a Pd-Ni(OH) catalyst. Notably, stable electrolysis over 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental and theoretical results reveal that 1) the OH* generation promoted by Ni(OH) plays a critical role in facilitating EG-to-GA oxidation and removing poisonous carbonyl species, thereby achieving high activity and stability; 2) Pd with a downshifted d-band center and the oxophilic Ni can synergistically facilitate the rapid desorption and transfer of GA from the active Pd sites to the inactive Ni sites, avoiding over-oxidation and thus achieving high selectivity.
电重整聚对苯二甲酸乙二醇酯衍生（PET 衍生）乙二醇（EG）为精细化学品和 H 是解决严重塑料污染的理想解决方案。在这里，我们报告了在 Pd-Ni(OH)催化剂上，即使在工业级电流密度（600mAcm-2，1.15V vs. RHE）下，EG 电氧化为羟基乙酸（GA）具有高法拉第效率和选择性（>85%）。值得注意的是，可实现超过 200 小时的稳定电解，优于所有可用的 Pd 基催化剂。实验和理论结果的结合表明：1）由 Ni(OH)促进的 OH*生成在促进 EG 到 GA 氧化和去除有毒羰基物种方面起着关键作用，从而实现了高活性和稳定性；2）具有下移位 d 带中心的 Pd 和亲氧 Ni 可以协同促进 GA 从活性 Pd 位快速解吸和转移到非活性 Ni 位，避免过度氧化，从而实现高选择性。
