首页|期刊导航|燃料化学学报(中英文)|焙烧气氛精准调控的Cu/SiO2催化剂用于高效催化丁二酸二甲酯加氢制1,4-丁二醇

焙烧气氛精准调控的Cu/SiO2催化剂用于高效催化丁二酸二甲酯加氢制1,4-丁二醇OA

Calcination atmosphere-engineered Cu/SiO2 catalysts for efficient hydrogenation of dimethyl succinate to 1,4-butanediol

中文摘要英文摘要

生物质衍生的丁二酸二甲酯催化加氢制备1,4-丁二醇,是绿色化学背景下生产高附加值C4化学品的一条关键路径.Cu/SiO2催化剂虽以酯加氢高选择性著称,但其性能本质上与铜物种的微观结构密切相关.尽管焙烧是形成催化剂活性结构的关键步骤,但焙烧气氛对其影响的系统性研究尚不充分.本研究采用尿素辅助水热法制备了 Cu/SiO2催化剂,并在不同气氛下进行焙烧,以阐明焙烧气氛对催化剂理化性质及其后续加氢性能的影响.通过N2物理吸脱附、FT-IR、H2-TRR、XRD、TEM、N2O化学吸附、XPS和NH3-TPD表征发现,焙烧气氛能显著改变金属-载体间相互作用,进而有效调控负载铜物种的分散度和化学状态.尤其是,在空气中焙烧后的催化剂,其金属-载体间相互作用较强,有效提高了铜物种的分散度,并增加了关键活性位Cu+的占比.在优化的反应条件下,Cu/SiO2-A催化剂展现了优异的催化性能,丁二酸二甲酯转化率达92.37%,1,4-丁二醇收率达64.15%.本工作证实了焙烧气氛工程是一种优化多相催化剂中金属-载体相互作用,从而实现高效加氢过程的强效策略.

The catalytic hydrogenation of biomass-derived dimethyl succinate(DMS)to 1,4-butanediol(BDO)represents a pivotal route for producing high-value C4 chemicals in the context of green chemistry.Cu/SiO2 catalysts are known for their high selectivity in hydrogenating ester groups,and their performance is correlated with the microstructure of the copper species.Although calcination is a critical step in defining this active structure,the systematic influence of the calcination atmosphere remains underexplored.In this study,Cu/SiO2 catalysts were prepared via a urea-assisted hydrothermal method and calcined under different atmospheres to elucidate their effects on catalyst physicochemical properties and subsequent hydrogenation performance.A comprehensive characterization suite(N2 physisorption,FT-IR,H2-TPR,XRD,TEM,N2O pulse chemisorption,XPS and NH3-TPD)revealed that the calcination atmosphere profoundly alters the metal-support interaction,thereby regulating the dispersion and chemical state of the loaded copper species.Specifically,calcination in air promoted a stronger metal-support interaction,effectively enhancing the dispersion of copper species and increasing the proportion of key active Cu+species.Consequently,the air-calcined catalyst demonstrated superior performance,achieving 92.37%DMS conversion and 64.15%BDO yield under optimized conditions(210 ℃,5.0 MPa,WHSV of 0.6 h-1,H2/DMS molar ratio of 100).This work underscores calcination atmosphere engineering as a potent strategy for optimizing metal-support interactions in heterogeneous catalysts for efficient hydrogenation processes.

邵旭浩;张旭妍;陈晓荣;杜嘉欣;艾培培;谭明慧;高志华;黄伟

太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024青岛科技大学材料科学与工程学院,山东青岛 266042青岛科技大学化工学院,山东青岛 266042太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024太原理工大学化学与化工学院省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024

化学化工

铜基催化剂焙烧气氛金属-载体相互作用加氢

copper-based catalystcalcination atmospheremetal-support interactionhydrogenation

《燃料化学学报(中英文)》 2026 (8)

232-242,11

Supported by National Natural Science Foundation of China(22008166)and Fundamental Research Program of Shanxi Province(202403021211029,201901D211047).

10.1016/S1872-5813(26)60663-9

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