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Cu-Based Catalysts Design Toward Electrochemical CO2 Reduction to Valuable Multi-Carbons Products 认领 引用
1
作者 Li‑Qing Li Min‑Xiao Huang +3 位作者 Hong Ke Wei‑Wei Zhu Jing‑Hua Zhao Li‑Hua Zhu 《Rare Metals》 SCIE EI CAS CSCD 2026年第4期284-303,共20页
Electrochemical reduction of CO2 to multi-carbon products(e.g.,C2+ ,ethene,ethanol,etc.)not only effectively decreases the CO2 concentration in atmosphere but also shows great potential economic benefits due ... Electrochemical reduction of CO2 to multi-carbon products(e.g.,C2+ ,ethene,ethanol,etc.)not only effectively decreases the CO2 concentration in atmosphere but also shows great potential economic benefits due to these exploitable value-added products.The Cu-based catalysts have caught much attention in CO2 electroreduction due to the good selectivity to hydrocarbons products.However,designing appropriate Cu-based catalysts is desirable to further improve the energy efficiency and selectivity of specific C2+ product.In this review,primary pathways of CO2 electroreduction to C2+ products are first discussed to summarize the key elementary steps of C2+ products formation.Subsequently,various strategies of catalytic activity regulation of Cu-based catalysts are classified into geometric and electronic structures modification based on the inner correlation between these strategies and the mechanism of C2+ products formation.The review ends with a cross-scale perspective that links the selectivity enhancement of a specific C2+ product and the target design of Cu-based catalysts. 展开更多
关键词 catalytic activity regulation Cu‑based catalysts electrochemical CO2reduction
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Promotional effect of cerium and niobium doping on Cu/TiO2 catalyst for diethylamine catalytic degradation 认领 引用
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作者 Xiaoqiang Wang Ling Zhou +1 位作者 Yue Liu Zhongbiao Wu 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第1期213-219,共7页
In this study,the promotional effect of Ce and Nb doping on Cu/TiO2 catalyst for diethylamine catalytic degradation was investigated.The activity tests reveal that the Ce and Nb modification can facilitate the risi... In this study,the promotional effect of Ce and Nb doping on Cu/TiO2 catalyst for diethylamine catalytic degradation was investigated.The activity tests reveal that the Ce and Nb modification can facilitate the rising of mineralization rate and N2 selectivity during diethylamine degradation,achieving over 90%mineralization rate at 250-450°C,along with N2 selectivity exceeding 80% within 300-400°C.Characterization results show that the co-addition of Ce and Nb induces strong interactions with Cu species and increases surface Brønsted acid sites.Crucially,the enhanced redox capability derived from interactions guarantees good catalytic activity and mineralization rate.Additionally,the increased Brønsted acidity from Nb doping can suppress the formation of NCO(a)species,resulting in less generation of NOx from NCO(a)oxidation.Moreover,the enhanced Brønsted acidity can promote the internal SCR reaction,which also reduces the NOx emission.This work could offer valuable insights for designing catalysts with superior catalytic performance for amine-like volatile organic compounds(VOCs)degradation. 展开更多
关键词 Catalytic degradation Diethylamine Cu/TiO2catalysts Cerium and niobium modification VOCs Rare earths
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草酸二甲酯加氢过程中Cu/SiO2催化剂失活机制研究 认领 引用
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作者 杜佳奇 李文龙 +5 位作者 王佳杰 宋元江 王小莉 赵安民 李扬 胡志彪 《低碳化学与化工》 CAS 北大核心 2026年第5期54-60,103,共7页
草酸二甲酯加氢制乙二醇是煤炭高效清洁利用的代表性技术路线,在“碳中和”背景下受到了广泛关注。尽管该路线已实现工业化,但在目前的工业装置中仍存在催化剂易失活的问题。为研究催化剂失活机制,选取Cu/SiO2催化剂为模型催化剂,通... 草酸二甲酯加氢制乙二醇是煤炭高效清洁利用的代表性技术路线,在“碳中和”背景下受到了广泛关注。尽管该路线已实现工业化,但在目前的工业装置中仍存在催化剂易失活的问题。为研究催化剂失活机制,选取Cu/SiO2催化剂为模型催化剂,通过稳定性评价测试,结合XRD、TEM、N2吸/脱附、TGA及XPS等表征方法,分析了煅烧、还原和失活Cu/SiO2催化剂催化性能和结构的变化。结果表明,导致Cu/SiO2催化剂失活的主要原因是Cu颗粒团聚、积炭及活性组分Cu的价态变化。其中,Cu颗粒团聚会导致暴露催化剂表面的活性位点数量减小,催化活性降低;中间产物发生一系列副反应产生的积炭会覆盖催化剂的部分活性位点,导致催化活性降低;反应过程中Cu的价态变化会导致Cu+和Cu0在催化加氢过程中的协同作用被破坏,导致催化剂失活。 展开更多
关键词 草酸二甲酯 加氢 乙二醇 Cu/SiO2催化剂 失活
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草酸二甲酯加氢制乙二醇Cu/SiO2基催化剂研究进展 认领 引用
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作者 王佳杰 李文龙 +5 位作者 赵安民 李扬 胡志彪 杜佳奇 宋元江 王小莉 《低碳化学与化工》 CAS 北大核心 2026年第6期37-51,共15页
煤制乙二醇(EG)路线是我国煤炭清洁高效利用战略的核心技术之一,草酸二甲酯(DMO)加氢制EG是煤制EG路线的关键步骤。Cu/SiO2基催化剂因其良好的催化性能和可控的成本实现了在DMO加氢制EG中的工业化应用。然而,现有技术还存在H2循... 煤制乙二醇(EG)路线是我国煤炭清洁高效利用战略的核心技术之一,草酸二甲酯(DMO)加氢制EG是煤制EG路线的关键步骤。Cu/SiO2基催化剂因其良好的催化性能和可控的成本实现了在DMO加氢制EG中的工业化应用。然而,现有技术还存在H2循环能耗大、催化剂寿命短等问题。首先,介绍了DMO加氢反应路径、催化剂活性位点与构效关系和失活机理。然后,从构效关系和工业应用角度出发,对复合制备工艺、助剂改性和催化剂微观-介观结构设计等活性中心调控策略进行了分析。最后,对用于DMO加氢制EG的Cu/SiO2基催化剂的未来发展进行了展望,如研究催化剂表面物种的动态演变及失活机理、寻找更有效的活性中心调控指标和研制适应低n(H2)(DMO)的Cu/SiO2基催化剂及其配套工艺。 展开更多
关键词 乙二醇 草酸二甲酯 Cu/SiO2基催化剂 反应机理 活性中心调控
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老化处理促进Cu/SiO2原位还原增强糠醛加氢制糠醇反应性能 认领 引用
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作者 高雯雯 梁越 +1 位作者 王金山 王康军 《低碳化学与化工》 CAS 北大核心 2026年第5期36-45,共10页
将生物质衍生物糠醛通过选择加氢转化为糠醇是实现生物质资源转化利用的重要途径之一。Cu/SiO2催化剂是工业领域常用加氢催化剂,但其在糠醛加氢反应中仍存在催化活性不足的问题。采用共沉淀法制备了Cu/SiO2催化剂,然后分别在常温... 将生物质衍生物糠醛通过选择加氢转化为糠醇是实现生物质资源转化利用的重要途径之一。Cu/SiO2催化剂是工业领域常用加氢催化剂,但其在糠醛加氢反应中仍存在催化活性不足的问题。采用共沉淀法制备了Cu/SiO2催化剂,然后分别在常温、60℃、80℃、100℃和120℃下进行老化处理,研究了老化温度对Cu/SiO2催化剂糠醛加氢制糠醇催化性能的影响,并分析了反应前后催化剂的结构变化情况。结果表明,在20 mL糠醛、催化剂用量为0.2 g、反应温度为180℃、反应压力为3.5 MPa和反应时间为2 h的最佳反应条件下,60℃下老化所得催化剂(Cu/SiO2(60))表现出良好的催化性能,其糠醛转化率为99.0%,糠醇选择性为96.2%。适宜的老化温度(60℃)可有效促进Cu2+物种在反应过程中原位还原为Cu0、Cu+物种,这有助于提高Cu物种分散性,减小Cu物种尺寸,从而提高催化剂催化性能。 展开更多
关键词 Cu/SiO2催化剂 老化温度 糠醛加氢 原位还原
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Cu/SiO2催化剂的制备及其乙醇脱氢制乙醛性能 认领 引用
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作者 魏浩宇 李晓晨 +4 位作者 苏振宇 王春雪 宋诗鹏 王国玮 祝晓琳 《石化技术与应用》 CAS 2026年第1期8-12,19,共5页
分别采用NH3蒸发法和浸渍法制备了一系列Cu/SiO2催化剂,利用X射线粉末衍射仪、全自动多用吸附仪、物理吸附仪、透射电子显微镜等仪器对上述催化剂进行了表征,考察了催化剂制备参数和反应条件对乙醇脱氢反应性能的影响。结果表明:... 分别采用NH3蒸发法和浸渍法制备了一系列Cu/SiO2催化剂,利用X射线粉末衍射仪、全自动多用吸附仪、物理吸附仪、透射电子显微镜等仪器对上述催化剂进行了表征,考察了催化剂制备参数和反应条件对乙醇脱氢反应性能的影响。结果表明:相比浸渍法,NH3蒸发法制备的催化剂的活性组分金属Cu分散得更均匀,在乙醇脱氢反应中呈现出更高的催化活性;NH3蒸发法制备的催化剂在Cu负载量(质量分数)为5%,反应温度为320℃,进料质量空速为2 h-1的优化条件下,乙醇转化率约为85.0%,乙醛选择性高于95.0%,且在60 h内呈现出良好的反应稳定性。 展开更多
关键词 Cu/SiO2催化剂 制备方法 NH3蒸发法 金属负载量 乙醇脱氢 乙醛 稳定性 选择性
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High Activity and Selectivity of Cu/SiO_2 Catalyst for the Direct Synthesis of Indole 认领 引用 被引量：3
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作者 Lei SHI Jun Ming SUN +2 位作者 Xin Ping WANG Xan Yun SU Tian Xi CAI 《Chinese Chemical Letters》 SCIE CAS 2002年第3期211-212,共2页
Copper supported over silica exhibited very high activity and selectivity for the direct synthesis of indole at atmospheric pressure. Under the reaction temperature of 325C,the yield of indole could obtain 88%.
关键词 Cu/SiO2 catalyst direct synthesis of indole aniline ethylene glycol.
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Cu-ZnO催化CO2加氢制甲醇反应构效关系研究进展 认领 引用 被引量：1
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作者 魏新煜 苏暐光 +3 位作者 白永辉 宋旭东 吕鹏 于广锁 《石油学报（石油加工）》 EI CAS CSCD 北大核心 2026年第1期107-117,共11页
CO2转化为甲醇可缓解温室效应并满足能源需求,而高效转化的关键在于催化剂设计。Cu-ZnO催化剂具有高转化率、良好甲醇选择性、低成本和易调控组成等优点,成为CO2加氢制甲醇的主流催化体系。从甲酸盐路径和逆水煤气变换路径2种反... CO2转化为甲醇可缓解温室效应并满足能源需求,而高效转化的关键在于催化剂设计。Cu-ZnO催化剂具有高转化率、良好甲醇选择性、低成本和易调控组成等优点,成为CO2加氢制甲醇的主流催化体系。从甲酸盐路径和逆水煤气变换路径2种反应路径综述了不同Cu-ZnO催化剂上CO2加氢制甲醇的研究进展,并对加氢反应中所涉及的活性位点及构效关系,如金属价态、界面相互作用、尺寸效应与限域效应等方面进行分析探讨。总结了近年来利用金属有机框架、分子筛、层状双金属氢氧化物和类水滑石化合物等材料制备的新型结构Cu-ZnO、Cu-ZnO-MxOy复合三元催化剂的甲醇生成活性。Cu基催化剂的活性和稳定性仍需提升,且反应中的关键中间体尚不明确,未来Cu-ZnO催化剂的研究应聚焦于原位分析与机器学习相结合,优化催化剂尺寸、形状及载体性能,整合酸碱与氧化还原功能,明确CO2转化机理并提高催化效率。 展开更多
关键词 Cu-ZnO催化剂 CO2加氢制甲醇 反应机理 活性位点 构效关系
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Cu负载量对Cu/CeO2催化CO2加氢制甲醇性能的影响 认领 引用
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作者 李传 谭延芹 +6 位作者 甘泽 何欣颖 张世博 粟子凌 罗辉 邓文安 杜峰 《中国石油大学学报（自然科学版）》 EI CAS CSCD 北大核心 2026年第2期202-210,共9页
研究Cu负载量为10%、20%及30%的Cu/CeO2催化剂对CO2加氢制甲醇性能的影响,采用XRD、BET和CO2-TPD等表征手段,分析Cu负载量对催化剂加氢性能影响的机制。结果表明:Cu负载量(质量分数)为20%的催化剂活性最佳,其在反应温度为240... 研究Cu负载量为10%、20%及30%的Cu/CeO2催化剂对CO2加氢制甲醇性能的影响,采用XRD、BET和CO2-TPD等表征手段,分析Cu负载量对催化剂加氢性能影响的机制。结果表明:Cu负载量(质量分数)为20%的催化剂活性最佳,其在反应温度为240℃、反应压力为3 MPa、质量空速为12000 mL/(g·h)以及V(H 2)/V(CO2)=3∶1时,CH3OH的选择性和时空收率为85.2%和13.8 g/(kg·h);Cu负载量为20%的催化剂呈现最小CeO2晶格参数和晶粒尺寸,比表面积最大,碱性活性位点数量最多,说明适宜的Cu负载量可增强Cu物种在CeO2载体表面的分散度,增大反应原料与催化剂的接触面积,提高催化剂对CO2分子的吸附能力,从而实现CO2加氢制甲醇反应中Cu/CeO2催化剂催化性能的提升。 展开更多
关键词 Cu负载量 Cu/CeO2催化剂 CO2加氢制甲醇 催化剂结构 机制
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In_2O_3-modified Cu/SiO_2 as an active and stable catalyst for the hydrogenation of methyl acetate to ethanol 认领 引用 被引量：11
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作者 Yu Zhang Chenliang Ye +2 位作者 Cuili Guo Changna Gan Xinmeng Tong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第1期99-108,共10页
A series of indium oxide‐modified Cu/SiO2catalysts were synthesized and used to produce ethanol via methyl acetate hydrogenation.In‐Cu/SiO2catalyst containing1.0wt%In2O3exhibited the best catalytic activity and stab... A series of indium oxide‐modified Cu/SiO2catalysts were synthesized and used to produce ethanol via methyl acetate hydrogenation.In‐Cu/SiO2catalyst containing1.0wt%In2O3exhibited the best catalytic activity and stability.The physicochemical properties of the synthesized catalysts were investigated using several characterization methods and the results showed that introducing suitable indium to Cu/SiO2increased the copper dispersion,diminished the copper crystallite size,and enriched the surface Cu+concentration.Furthermore,the Cu/SiO2catalyst gradually deactivated during the stability test,which was mainly attributed to copper sintering and the valence change in surface copper species.In contrast,indium addition can inhibit the thermal transmigration and accumulation of copper nanoparticles to stabilize the catalyst.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved. 展开更多
关键词 Methyl acetate Hydrogenation Indium Cu/SiO2 catalyst Ethanol
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Utilization of steelwork off-gases through methanol synthesis:Sulfur-induced dynamic migration of ZnOx over industrial Cu/ZnO/Al2O3 catalyst and the poisoning mechanism 认领 引用
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作者 Yukun Tian Yu Zeng +5 位作者 Ziyang Chen Hua Tong Ming Chen Zhiyong Zhong Daiqi Ye Limin Chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2025年第12期659-673,共15页
The reduction of carbon emissions in the steel industry is a significant challenge,and utilizing CO2 from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonizatio... The reduction of carbon emissions in the steel industry is a significant challenge,and utilizing CO2 from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonization.However,steelwork off-gases typically contain various impurities,including H2S,which can deactivate commercial methanol synthesis catalysts,Cu/ZnO/Al2O3(CZA).Reverse water-gas shift(RWGS)reaction is the predominant side reaction in CO2 hydrogenation to methanol which can occur at ambient pressure,enabling the decouple of RWGS from methanol production at high pressure.Then,a series of activated CZA catalysts has been in-situ pretreated in 400 ppm H2S/Ar at 250℃and tested for both RWGS reaction at ambient pressure and CO2 hydrogenation to methanol at high pressure.An innovative decoupling strategy was employed to isolate the RWGS reaction from the methanol synthesis process,enabling the investigation of the evolution of active site structures and the poisoning mechanism through elemental analysis,X-ray Diffraction,X-ray Photoelectron Spectroscopy,Fourier Transform Infrared Spectroscopy,Temperature Programmed Reduction and CO2 Temperature Programmed Desorption.The results indicate that there are different dynamic migration behaviors of ZnOx in the two reaction systems,leading to different poisoning mechanisms.These interesting findings are beneficial to develop sulfur resistant and durable highly efficient catalysts for CO2 hydrogenation to methanol,promoting the carbon emission reduction in steel industry. 展开更多
关键词 Steelwork off-gases CO2hydrogenation to methanol H2S Cu/Zn O/Al2O3catalysts ZnOxmigration Deactivation and promotion mechanisms
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Theoretical Study of Dehydrogenation Reaction Mechanism on Cu10/TiO2,Au10/TiO2,Au8Cu2/TiO2,or Cu1/Au8Cu2/TiO2Surfaces 认领 引用
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作者 Hongwei Li Ruimin Wang +2 位作者 Caifang Han Bo Ren Hongjun Fan 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2026年第2期225-232,I0069-I0071,I0170,共8页
Comprehensive analysis of the connection be-tween surface metal species and the mechanism of hydrogen(H2)generation on TiO2provides important new information for the develop-ment of more effective catalysts for ... Comprehensive analysis of the connection be-tween surface metal species and the mechanism of hydrogen(H2)generation on TiO2provides important new information for the develop-ment of more effective catalysts for H2 produc-tion.We have systematically investigated the mechanism of catalytic H2 generation on the Cu10/TiO2,Au10/TiO2,Au8Cu2/TiO2and Cu1/Au8Cu2/TiO2surfaces using density func-tional theory.Our results demonstrate an O-Hδ+···Hδ−-M type transition state for H2 production,and the Au8Cu2(0.54 eV)bimetal-lic cluster catalyst exhibits more activity in comparison to the Cu10(0.63 eV)and Au10(0.88 eV)cluster catalysts on the TiO2surface.On the Cu1/Au8Cu2/TiO2surface,we found that Au8Cu2clusters act as electron donors,while Cu single atom acts as an electron acceptor.Therefore,the Au8Cu2bimetallic catalyst has a low energy barrier(0.58 eV)in the reductive reaction of H2 production in water,but Cu single atom as the catalytic center has a higher en-ergy barrier(1.49 eV).This implies that bimetallic catalysts may be able to catalyze the wa-ter dehydrogenation reaction more successfully,which would be important knowledge for comprehending and refining the photocatalytic H2 generation process. 展开更多
关键词 TiO2surface Metal cluster Dehydrogenation Cu Au Bimetallic catalyst Den-sity functional theory
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Effect of copper loading on texture,structure and catalytic performance of Cu/SiO_2 catalyst for hydrogenation of dimethyl oxalate to ethylene glycol 认领 引用 被引量：15
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作者 Bo Zhang Shengguo Hui +3 位作者 Suhua Zhang Yang Ji Wei Li Dingye Fang 《Journal of Natural Gas Chemistry》 CSCD 2012年第5期563-570,共8页
Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation （UHDP） technique have been proposed focusing on the effect of copper loading.The texture,structure a... Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation （UHDP） technique have been proposed focusing on the effect of copper loading.The texture,structure and composition are systematically characterized by ICP,FTIR,N 2-physisorption,N2O chemisorption,TPR,XRD and XPS.The formation of copper phyllosilicate is observed in Cu/SiO2 catalyst by adopting UHDP method,and the amount of copper phyllosilicate is related to copper loading.It is found the structure properties and catalytic performance is profoundly affected by the amount of copper phyllosilicate.The excellent catalytic activity is attributed to the synergetic effect between Cu0 and Cu ＋.DMO conversion and EG selectivity are determined by the amount of Cu0 and Cu＋,respectively.The proper copper loading （30 wt%） provides with the highest ratio of Cu ＋ /Cu0,giving rise to the highest EG yield of 95% under the reaction conditions of p=2.0 MPa,T=473 K,H2/DMO=80 and LHSV=1.0h-1. 展开更多
关键词 Cu/SiO2 copper loading dimethyl oxalate ethylene glycol copper phyllosilicate
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Effects of ethanol on the in situ synthesized Cu/SiO2catalyst:Texture,structure,and the catalytic performance in hydrogenation dimethyl oxalate to ethylene glycol 认领 引用 被引量：6
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作者 Shu Rong Wang Ling Jun Zhu +2 位作者 Ying Ying Zhu Xiao Lan Ge Xin Bao Li 《Chinese Chemical Letters》 SCIE CAS CSCD 2011年第3期362-365,共4页
The Cu/SiO2catalysts were in situ synthesized by the hydrolysis of tetraethyl orthosilicate(TEOS)in one phase solution using ethanol as co-solvent or TEOS/H_2O two phases solution,followed by the precipitation of c... The Cu/SiO2catalysts were in situ synthesized by the hydrolysis of tetraethyl orthosilicate(TEOS)in one phase solution using ethanol as co-solvent or TEOS/H_2O two phases solution,followed by the precipitation of copper on SiO2by ammonia evaporation.In the hydrogenation of dimethyl oxalate,the catalyst prepared by one phase hydrolysis exhibited higher activity and ethylene glycol(EG)selectivity at lower temperature than that of two phases due to its larger BET surface area and multimodal pore distribution.At 488-503 K,the catalyst prepared in one phase solution with water/ethanol(W/E)volume ratio of 3:1 exhibited 90-95%EG selectivity,while catalyst prepared by two phase hydrolysis reached 90%EG selectivity only at 498-503 K. 展开更多
关键词 Ethanol Cu/SiO2 TEOS Hydrogenation Dimethyl oxalate Ethylene glycol
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An efficient and stable Cu/SiO_2 catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate 认领 引用 被引量：10
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作者 Jiaju Liu Peng He +3 位作者 Liguo Wang Hui Liu Yan Cao Huiquan Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第8期1283-1293,共11页
The efficient synthesis of methanol and ethylene glycol via the chemoselective hydrogenation of ethylene carbonate（EC） is important for the sustainable utilization of CO_2 to produce commodity chemicals and fuels. I... The efficient synthesis of methanol and ethylene glycol via the chemoselective hydrogenation of ethylene carbonate（EC） is important for the sustainable utilization of CO_2 to produce commodity chemicals and fuels. In this work, a series of β-cyclodextrin-modified Cu/SiO_2 catalysts were prepared by ammonia evaporation method for the selective hydrogenation of EC to co-produce methanol and ethylene glycol. The structure and physicochemical properties of the catalysts were characterized in detail by N_2 physisorption, XRD, N_2O titration, H_2-TPR, TEM, and XPS/XAES. Compared with the unmodified 25 Cu/SiO_2 catalyst, the involvement of β-cyclodextrin in 5β-25 Cu/SiO_2 could remarkably increase the catalytic activity—excellent activity of 1178 mgEC g_（cat）^（–1） h^（–1） with 98.8%ethylene glycol selectivity, and 71.6% methanol selectivity could be achieved at 453 K. The remarkably improved recyclability was primarily attributed to the remaining proportion of Cu~＋/（Cu^0＋Cu~＋）. Furthermore, the DFT calculation results demonstrated that metallic Cu^0 dissociated adsorbed H_2, while Cu~＋ activated the carbonyl group of EC and stabilized the intermediates. This study is a facile and efficient method to prepare highly dispersed Cu catalysts—this is also an effective and stable heterogeneous catalyst system for the sustainable synthesis of ethylene glycol and methanol via indirect chemical utilization of CO_2. 展开更多
关键词 Ethylene carbonate Hydrogenation β-Cyclodextrin Cu/SiO2 Methanol Ethylene glycol
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Zr(Ⅳ) surface sites determine CH3OH formation rate on Cu/ZrO2/SiO2-CO2 hydrogenation catalysts 认领 引用 被引量：3
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作者 Erwin Lam Kim Larmier +3 位作者 Shohei Tada Patrick Wolf Olga V. Safonova Christophe Copéret 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第11期1741-1748,共8页
Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carri... Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carried out on the Cu and Zr K-edge. Under reaction conditions, Cu remains metallic, while Zr is present in three types of coordination environment associated with 1) bulk ZrO2, 2) coordinatively saturated and 3) unsaturated Zr(Ⅳ) surface sites. The amount of coordinatively unsaturated Zr surface sites can be quantified by linear combination fit of reference X-Ray absorption near edge structure (XANES) spectra and its amount correlates with CH3OH formation rates, thus indicating the importance of Zr(Ⅳ) Lewis acid surface sites in driving the selectivity toward CH3OH. This finding is consistent with the proposed mechanism, where CO2 is hydrogenated at the interface between the Cu nanoparticles that split H2 and Zr(Ⅳ) surface sites that stabilizes reaction intermediates. 展开更多
关键词 CO2 hydrogenation ZrO2/SiO2 supported Cu nanoparticles Lewis acidic surface sites In situ X-ray absorption spectroscopy
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Catalytic Performance and Texture of TEOS Based Cu/SiO2Catalysts for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol 认领 引用 被引量：3
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作者 WANG Shu-rong YIN Qian-qian LI Xin-bao 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 2012年第1期119-123,共5页
Highly active and selective Cu/SiO2catalysts for hydrogenation of dimethyl oxalate(DMO)to ethylene glycol(EG)were successfully prepared by means of a convenient one-pot synthetic method with tetraethoxysi lane(TEOS... Highly active and selective Cu/SiO2catalysts for hydrogenation of dimethyl oxalate(DMO)to ethylene glycol(EG)were successfully prepared by means of a convenient one-pot synthetic method with tetraethoxysi lane(TEOS)as the source of silica.XRD,H2-TPR,SEM,TEM,XRF and N2 physisorption measurements were performed to characterize the texture and structure of Cu/SiO2catalysts with different copper loadings.The active components were highly dispersed on SiO2supports.Furthermore,the coexistence of CuO and Cu+contributed a lot to the excellent performance of Cu-TEOS catalysts.The DMO conversion reached 100%and the EG selectivity reached 95%at 498 K and 2 MPa with a high liquid hourly space velocity over the 27-Cu-TEOS catalyst with an actual cop per loading of 19.0%(mass fraction). 展开更多
关键词 Cu/SiO2 TEOS Hydrogenation Dimethyl oxalate Ethylene glycol
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Synthesis of Methyl Glycolate by Hydrogenation of Dimethyl Oxalate over Cu-Ag/SiO_2 Catalyst 认领 引用 被引量：26
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作者 Baowei Wang Qian Xu Hua Song Genhui Xu 《Journal of Natural Gas Chemistry》 2007年第1期78-80,共3页
Methyl glycolate is a good solvent and can be used as feedstock for the synthesis of some important organic chemicals. Catalytic hydrogenation of dimethyl oxalate （DMO） over copper-silver catalyst supported on silic... Methyl glycolate is a good solvent and can be used as feedstock for the synthesis of some important organic chemicals. Catalytic hydrogenation of dimethyl oxalate （DMO） over copper-silver catalyst supported on silica was studied. The Cu-Ag/SiO2 catalyst supported on silica sol was prepared by homogeneous deposition-precipitation of the mixture of aqueous euprammonia complex and silica sol. The proper active temperature of Cu-Ag/SiO2 catalyst for hydrogenation of DMO was 523-623 K. The most preferable reaction conditions for methyl glycolate （MG） were optimized： temperature at 468-478 K, 40-60 mesh catalyst diameter, H2/DMO ratio 40, and 1.0 h^-1 of LHSV. 展开更多
关键词 dimethyl oxalate methyl glycolate ethylene glycol hydrogenation Cu-Ag/SiO2 catalyst
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In situ IR study of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO_2 catalyst 认领 引用 被引量：2
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作者 Shengguo Hui Bo Zhang +1 位作者 Suhua Zhang Wei Li 《Journal of Natural Gas Chemistry》 CSCD 2012年第6期753-758,共6页
The mechanism of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst was investigated by in situ Fourier transform infrared （FTIR） spectroscopy. It was found that dimethyl oxalate and methyl glyc... The mechanism of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst was investigated by in situ Fourier transform infrared （FTIR） spectroscopy. It was found that dimethyl oxalate and methyl glycolate proceeded via dissociative adsorption on Cu/SiO2 catalyst, and four main intermediates, CH3OC（O）（O）C-M （1655 cm-1）, M-C（O）（O）C-M （1618 cm-1）, HOCH2（O）C--M （1682 cm-1） and CH3O-M （2924-2926 cm-1）, were identified during the reaction. It was concluded that dimethyl oxalate hydrogenation to ethylene glycol mainly proceeded along the route： dimethyl oxalate ／rightarrow CH3OC（O）（O）C-M → methyl glycolate →HOCH2（O）C-M → ethylene glycol. Finally a schematic reaction network was proposed. 展开更多
关键词 dimethyl oxalate ethylene glycol FTIR hydrogenation Cu/SiO2
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CO2加氢制甲醇Cu基催化剂研究进展 认领 引用
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作者 于跃 陈利达 +4 位作者 王学波 陈晓 卢晓峰 杨阳 宋兰兰 《低碳化学与化工》 CAS 北大核心 2026年第7期25-44,共20页
CO2过度排放引起的气候变化,对人类的生存与发展构成了严重威胁。通过催化加氢将CO2转化为甲醇,既能实现碳资源的循环利用,又能缓解化石能源过度消耗引起的环境压力。Cu基催化剂具有良好的CO2加氢催化活性且成本较低,是目前CO_... CO2过度排放引起的气候变化,对人类的生存与发展构成了严重威胁。通过催化加氢将CO2转化为甲醇,既能实现碳资源的循环利用,又能缓解化石能源过度消耗引起的环境压力。Cu基催化剂具有良好的CO2加氢催化活性且成本较低,是目前CO2加氢制甲醇领域的研究热点之一。根据近年来CO2加氢制甲醇Cu基催化剂的研究情况,重点阐述了催化剂制备方法、活性位点构筑及酸碱性调控对催化剂催化活性的影响。然后,分析了反应过程中催化剂的失活路径,并总结了提升催化剂稳定性的策略。最后,对CO2加氢制甲醇Cu基催化剂的未来研究方向进行了展望。 展开更多
关键词 CO2加氢制甲醇 Cu基催化剂 活性位 酸碱调控
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