脱氢
化学
氢
催化作用
溢出效应
选择性
电子转移
化学工程
光化学
有机化学
工程类
经济
微观经济学
作者
Xuanlin Guo,Huifang Wu,Yang Zhao,Lirong Zheng,Qian Wang,Dianqing Li,Junting Feng
摘要
Abstract Acceptorless dehydrogenation of biomass‐alcohol provides an appealing route for co‐producing green H 2 and high‐value chemicals. However, the sluggish H species binding step severely inhibits reaction equilibrium and cause C‐C cleavage. Herein, we propose a unique directional H spillover strategy driven by controlling electron transport direction via constructing Au‐O‐Cu‐O‐Mg/Al interfacial structure, to allow H species transfer from O‐H dehydrogenation Cu 2+ site to C‐H dehydrogenation Au site to promote H 2 formation. The structure that each Cu precisely terminated by Mg/Al is inherited from layered double hydroxides with orderly dispersed atom arrangement. Comprehensive studies substantiate that the unreducible Mg 2+ /Al 3+ blocks electron transfer toward support, whereas Au‐O‐Cu electronic interaction drives H spillover from the support to Au. The Au/CuMgAl catalyst demonstrated unprecedentedly high glycerol dehydrogenation activity, showing 3–10 times turnover frequency (1.18 × 10 4 h −1 ) than other biomass‐derived H 2 formation system, co‐producing lactic acid with selectivity up to 98.8%.
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