高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

Cl-介导Fe/MgO-CaO晶面工程与电子结构协同调控催化甘油氢解

穆荣臻1,2, 王瑾1,2, 杨杰1,2, Roy Tania1,2, 汪杰1,2, 郭宝成1,2, 周春晖1,2
  

  1. 1. 绿色化学合成与转化技术全国重点实验室, 浙江工业大学化学工程学院 2. 安徽省国际交流合作基地, 青阳非金属矿研究院

  • 收稿日期:2025-12-23 修回日期:2026-03-15 网络首发:2026-04-22 发布日期:2026-04-22
  • 通讯作者: 周春晖 E-mail:clay@zjut.edu.cn
  • 基金资助:
    国家自然科学基金(批准号: 42572045, 22072136, W2433034)资助

Cl-Mediated Facet Engineering and Electronic Modulation of Fe/MgO-CaO Catalysts for Glycerol Hydrogenolysis

MU Rongzhen1,2, WANG Jin1,2, YANG Jie1,2, ROY Tania1,2, WANG Jie1,2, GUO Baocheng1,2, ZHOU Chunhui1,2*   

  1. 1. Research Group for Advanced Materials & Sustainable Catalysis (AMSC), State Key Laboratory of Green Chemical Synthesis and Conversion, College of Chemical Engineering, Zhejiang University of Technology 2. Anhui International Exchange and Cooperation Base, Qing Yang Institute for Industrial Minerals
  • Received:2025-12-23 Revised:2026-03-15 Online First:2026-04-22 Published:2026-04-22
  • Contact: Chunhui Zhou E-mail:clay@zjut.edu.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China (42572045, 22072136, W2433034)

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摘要： 针对传统浸渍法制备催化剂中活性组分易团聚, 高活性晶面难以定向暴露等问题, 本文提出了一种Cl-介导的晶体定向生长与电子结构等多重调控策略, 有效提升了Fe/MgO-CaO的催化性能. 研究结果表明, 在宏观形貌上, NH4Cl热解产生的气体刻蚀效应构建了催化剂的多孔特征, 并作为形貌调节剂诱导MgO-CaO由无序片状定向生长为(200)晶面择优暴露的棒状结构. 在微观物相上, Cl-的掺杂强化了Fe物种与MgO晶格的相互作用, 有效抑制了活性组分的团聚, 促使形成高分散的Mg-Fe-O固溶体, 此外, 还在催化剂表面衍生出均匀分布的Lewis酸位点. 且棒状固溶体结构在反应中表现出优异的稳定性, 有效避免了骨架坍塌. 当Fe-Cl摩尔比为1.00时, 甘油转化率较未掺杂的样品从60 %提 升至90 %. 本文采用的Cl?多重调控策略为天然矿物资源的高值化利用及高效非贵金属氧化物催化剂的设计提供了新的研究思路

关键词: 甘油, 过渡金属铁, Cl?, MgO/CaO, 1,2-丙二醇

Abstract: To overcome the limitations of active component aggregation and uncontrolled facet exposure typical of impregnation methods, we report a chloride-mediated engineering strategy to precisely tailor the morphology and electronic structure of Fe/MgO-CaO catalysts. Structural characterizations reveal that the gas-etching effect during NH?Cl pyrolysis creates a porous architecture. Acting as a morphological modifier, NH?Cl induces the directional growth of MgO-CaO from disordered sheets into a rod-like structure with preferentially exposed (200) facets. At the microstructural level, Cl- doping strengthens the interaction between Fe species and the MgO lattice. This effectively inhibits the agglomeration of active components and promotes the formation of a highly dispersed Mg-Fe-O solid solution, while generating uniformly distributed Lewis acid sites on the catalyst surface. Consequently, the unique rod-like solid solution exhibits excellent structural stability during the catalytic reaction, successfully preventing framework collapse. Consequently, the optimized catalyst (Fe-Cl = 1.00) boosted glycerol conversion from 60 % to 90 % relative to the Cl- free benchmark. This chloride-mediated engineering strategy provides a blueprint for valorizing natural minerals and rationally designing robust non-noble metal catalysts.

Key words: Glycerol; Transition metal iron, Chloride, MgO/CaO, 1,2-Propanediol

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