文献类型：期刊文献

英文题名：Interface-Engineered Electron-Deficient Nickel Species for Efficient Depolymerization of Polyethylene Terephthalate

作者：Xing, Sensen[1];Wang, Wenjie[1];Zhang, Xiangxue[1];Sun, Weixiao[1];Ge, Xiaohu[1];Zheng, Weizhong[1];Cao, Yueqiang[1];Chen, Wenyao[1];Qian, Gang[1];Duan, Xuezhi[1];Zhou, Xinggui[1];Chen, De[1,2];Zhang, Jing[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn & Low Carbon Technol, Shanghai, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, Trondheim, Norway

年份：2026

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20261820646166);WOS:【SCI-EXPANDED(收录号:WOS:001753952400001)】；

基金：This work was financially supported by National Natural Science Foundation of China (22378117 and 22408097), Fundamental and Interdisciplinary Disciplines Breakthrough Plan of the Ministry of Education of China (JYB2025XDXM404), China Postdoctoral Science Foundation General Program (2025M771163), Shanghai Huayi Holdings Group Co., Ltd., and the Guangxi Science and Technology Innovation Platform Program (LT2504240028). The authors thank the staff of beamlines BL16U1 (https://cstr.cn/31124.02.SSRF.BL16U1) and BL13SSW (https://cstr.cn/31124.02.SSRF.BL13SSW) at Shanghai Synchrotron Radiation Facility for experimental supports. The authors are also thankful to Professor J. Will Medlin from University of Colorado Boulder for helpful discussion.

语种：英文

外文关键词：depolymerization; heterogeneous catalysis; interface engineering; nickel; polyethylene terephthalate

摘要：Polyethylene terephthalate (PET) is the most abundant polyester plastic. Its chemical recycling mainly relies on homogeneous catalysis, often suffering from difficult catalyst separation and substantial waste generation. Previous work using heterogeneous catalysts has primarily focused on increasing Lewis acidity through variation of metal oxide types to improve performance, but catalyst activity remains limited. Here, we adopt an alternative strategy for modulating Lewis acidity with enhanced control by systematically tuning electronic properties of structurally versatile Ni active sites. Nickel can readily form intermetallics and layered double hydroxide (LDH) derivatives, providing substantial flexibility for modulating its electronic structure. We establish an electron-deficiency-dependent activity framework and discover a Ni3Ga/NiAlOx catalyst that exhibits unexpectedly high activity, surpassing more strongly Lewis-acidic fully oxidized Ni species and delivering an order-of-magnitude activity enhancement compared with conventional Lewis-acidic oxides. This high activity originates from electron-deficient interfacial Ni sites where electron withdrawal from O in LDH-derived NiAlOx and electron donation from Ga in intermetallic Ni3Ga result in appropriate Lewis acidity, enabling near-quantitative dimethyl terephthalate recovery from post-consumer PET. Theoretical and experimental validation suggests that such bidirectional electronic modulation balances substrate activation and product desorption, thereby maximizing catalytic efficiency. The catalyst is prepared via an industrially-established co-precipitation method and is readily scalable.