Concerted and Selective Electrooxidation of Polyethylene-Terephthalate-Derived Alcohol to Glycolic Acid at an Industry-Level Current Density over a Pd−Ni(OH)2 Catalyst
Fulai Liu, Xutao Gao, Rui Shi, Prof.?Dr. Zhengxiao Guo, Prof.?Dr. Edmund C. M. Tse, Prof.?Dr. Yong Chen
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引用次数: 10
Abstract
Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H2 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−2 at 1.15 V vs. RHE) over a Pd−Ni(OH)2 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)2 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酯(pet)衍生的乙二醇(EG)为精细化学品和氢气是解决严重塑料污染的理想方案。在这里,我们报道了在Pd - Ni(OH)2催化剂上,即使在工业级电流密度(600 mA cm - 2, 1.15 V vs. RHE)下,EG电氧化成乙醇酸(GA)也具有很高的法拉第效率和选择性(> 85%)。值得注意的是,可以实现超过200小时的稳定电解,优于所有现有的钯基催化剂。实验与理论相结合的结果表明:1)Ni(OH)2促进OH*生成在促进eg - ga氧化和去除有毒羰基物质中起着关键作用,从而获得高活性和稳定性;2) d带中心下移的Pd与亲氧Ni可协同促进GA从活性Pd位点快速解吸转移到非活性Ni位点,避免过度氧化,从而实现高选择性。
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.