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Pt-modulated Cu/SiO_(2) catalysts for efficient hydrogenation of CO_(2)-derived ethylene carbonate to methanol and ethylene glycol

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Chinese Journal of Chemical Engineering 2022年第1期35卷 366-373页

作者： Busha Assaba Fayisa Yushan Xi Youwei Yang Yueqi Gao Antai Li Mei-Yan Wang Jing Lv Shouying Huang Yue Wang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Zhejiang Institute of Tianjin University Ningbo 315201China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China

Copper-based catalysts were widely used in the heterogeneous selective hydrogenation of ethylene carbonate(EC),a key step in the indirect conversion of CO_(2) to ***,a high H_(2)/EC molar ratio in feed is required to achieve favorable activity and the methanol selectivity still needs to be ***,we fabricated a series of Pt-modulated Cu/SiO_(2) catalysts and investigated their catalytic performance for hydrogenation of EC in a fixed bed *** modulating the Pt amount,the optimal 0.2Pt-Cu/SiO_(2) catalyst exhibited the highest catalytic performance with99%EC conversion,over 98%selectivity to ethylene glycol and 95.8%selectivity to methanol at the H_(2)/EC ratio as low as 60 in *** addition,0.2Pt-Cu/SiO_(2) catalyst showed excellent stability for 150 h on stream over different H_(2)/EC ratios of *** is demonstrated a proper amount of Pt could significantly lower the H_(2)/EC molar ratio,promote the reducibility and dispersion of copper,and also enhance surface density of Cu+*** could be due to the strong interaction of Cu and Pt induced by formation of alloyed Pt single atoms on the Cu ***,a relatively higher amount of Pt would deteriorate the catalytic activity,which could be due to the surface coverage and aggregation of active *** findings may enlighten some fundamental insights for further design of Cu-based catalysts for the hydrogenation of carbon–oxygen bonds.

关键词： CO_(2) Ethylene carbonate Hydrogenation Pt-Cu/SiO_(2)catalyst Ethylene glycol Methanol

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Proximity Effect of Fe-Zn Bimetallic Catalysts on CO_(2) Hydrogenation Performance

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Transactions of Tianjin University 2023年第4期29卷 293-303页

作者： Shengkun Liu Qiao Zhao Xiaoxue Han Chongyang Wei Haoting Liang Yidan Wang Shouying Huang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education Haihe Laboratory of Sustainable Chemical TransformationsSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China School of materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Zhejiang Institute of Tianjin University Ningbo 315201China

The interaction between a promoter and an active metal crucially impacts catalytic ***,the influence of promoter contents and species has been intensively *** this study,we investigate the effect of the iron(Fe)-zinc(Zn)proximity of Fe-Zn bimetallic catalysts on CO_(2)hydrogenation *** eliminate the size effect,Fe_(2)O_(3)and ZnO nanoparticles with uniform size are first prepared by the thermal decomposition *** changing the loading sequence or mixing method,a series of Fe-Zn bimetallic catalysts with different Fe-Zn distances are *** with a series of characterization techniques and catalytic performances,Fe-Zn bimetallic proximity for compositions of Fe species is ***,we observe that a smaller Fe-Zn distance inhibits the reduction and carburization of the Fe species and facilitates the oxidation of *** proximity of Fe and Zn(i.e.,Fe_1Zn_(1)-imp and Fe_(1)Zn_(1)-mix samples)results in a suitable ratio of the Fe_5C_(2)and Fe_(3)O_(4)phases,simultaneously promoting the reverse water-gas shift and Fischer-Tropsch synthesis *** study provides insight into the proximity effect of bimetallic catalysts on CO_(2)hydrogenation performance.

关键词： CO_(2)hydrogenation Fe-based catalyst Promoter Proximity effect

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Enhanced synergy between Cu^(0) and Cu^(+) on nickel doped copper catalyst for gaseous acetic acid hydrogenation

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Frontiers of Chemical Science and Engineering 2021年第3期15卷 666-678页

作者： Jingwei Zhang Lingxin Kong Yao Chen Huijiang Huang Huanhuan Zhang Yaqi Yao Yuxi Xu Yan Xu Shengping Wang xinbin ma Yujun Zhao Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

As the substitution of common noble catalysts in the hydrogenation of carboxylic acid,a highly effective Cu-Ni/SiO_(2) catalyst was prepared by a novel stepwise ammonia evaporation *** performance in the gasphase hydrogenation of acetic acid was further *** the introduction of Ni dopant,more stable Cu^(δ+) sites,which can adsorb more acetic acid,were formed due to the electron transfer from Cu to *** makes more Cu^(0) sites available for hydrogen adsorption,which was suggested as the rate-determining step in acetic acid hydrogenation.A conversion of 99.6% was successfully achieved on this new Cu/SiO_(2)-0.5Ni catalyst,accompanied by the ethanol selectivity of 90%.The incorporation of nickel between copper nanoparticles enhances the synergistic effect between Cu^(0) and Cu^(+).It also helps mitigate the aggregation of copper nanoparticles due to the Ostwald ripening effect induced by acetic acid and enhance the stability of copper catalyst in the conversion of carboxylic acid.

关键词： carboxylic acid hydrogenation copper nickel stability

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Pd-Fe/a-AI203/cordierite monolithic catalysts for the synthesis of dimethyl oxalate： effects of calcination and structure

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Frontiers of Chemical Science and Engineering 2012年第3期6卷 259-269页

作者： Shengping WANG Xin ZHANG Yujun ZHAO Yadong GE Jing LV Baowei WANG xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Cordierite monoliths coated with Pd-Fe/a- Al2O3 catalysts were prepared at various calcination temperatures and characterized by thermogravimetry, temperature-programmed reduction, transmission electron microscopy, diffuse reflectance infrared Fourier transfor- mation spectroscopy and X-ray diffraction. The performance of the catalytic monoliths for the synthesis of dimethyl oxalate （DMO） through a CO coupling reaction was evaluated. Monolithic catalysts with calcination temperatures ranging from 473 K to 673 K exhibited excellent dispersion of Pd, good CO adsorption properties, and excellent performance for the coupling reaction. The optimized monolithic catalyst exhibited a much higher Pd efficiency （denoted as DMO （g）.Pd （g）-1 h 1）（733h-1） than that of the granular catalyst （60.2 h-1）, which can be attributed to its honeycomb structure and the large pore sizes in the a-Al2O3 washcoat which was accompanied with an even distribution of the active component in the coating layer along the monoliths channels.

关键词： dimethyl oxalate coupling Pd cordierite,monolith calcination structure

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Intermetallic CuAu nanoalloy for stable electrochemical CO_(2) reduction

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Chinese Chemical Letters 2023年第7期34卷 226-229页

作者： Siyu Kuang Minglu Li Xiaoyi Chen Haoyuan Chi Jianlong Lin Zheng Hu Shi Hu Sheng Zhang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Tianjin Key Laboratory of Molecular Optoelectronic Science School of ScienceTianjin UniversityTianjin 300072China

Copper is one of the most efficient catalysts widely investigated in electrochemical CO_(2) reduction, however, the further development of copper-based catalysts is constrained by severe stability problems. In this work, we developed a method for the synthesis of highly ordered Cu Au intermetallic nanoalloys(o-CuAu) under mild conditions(may provide insight into the rational design of stable CO_(2) RR electrocatalysts through proper structural engineering.

关键词： CO_(2)reduction CuAu nanoalloy Intermetallic Stability Electrocatalysts

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Enhanced selective hydrogenation of glycolaldehyde to ethylene glycol over Cu^(0)-Cu^(+)sites

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Chinese Journal of Chemical Engineering 2023年第5期57卷 141-150页

作者： Qi Yang Weikang Dai maoshuai Li Jie Wei Yi Feng Cheng Yang Wanxin Yang Ying Zheng Jie Ding Mei-Yan Wang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Selective hydrogenation of hydroxyaldehydes to polyalcohols is challenging due to the competitive hydrogenation of C=O and *** study develops heterogeneous Cu catalysts for the selective synthesis of ethylene glycol via batch liquid-phase hydrogenation of ***_(2)supported Cu,fabricated by ammonia evaporation,enables to catalyze the C=O bond hydrogenation with retaining the CAO bond intact,yielding higher selective hydrogenation activity with ethylene glycol selectivity up to 99.8%relative to MgO,Al_(2)O_(3),CeO_(2),and TiO_(2)supports and Cu/SiO_(2)synthesized by deposition–precipitation and *** confirm that highly efficient 20Cu/SiO_(2)-AE-623 K catalyst fabricated by ammonia evaporation is featured with larger Cu^(0)and Cu^(+)surface areas,of which the Cu^(+)species created from reducing copper phyllosilicate exhibit higher reactivity.A synergistic effect between Cu^(+)and Cu^(0)facilitates the selective adsorption/activation of glycolaldehyde on Cu^(+)sites and the dissociation of H_(2)on Cu^(0)sites,bringing a remarkable improvement in the selective hydrogenation performance.

关键词： Hydrogenation Multiphase reaction Biomass Copper phyllosilicate Ammonia evaporation

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Regulating electronic environment on alkali metal-doped Cu@NS-SiO_(2) for selective anisole hydrodeoxygenation

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绿色化学工程(英文) 2023年第3期4卷 294-302页

作者： Xiaofei Wang Xiaoxue Han Li Kang Shixiang Feng Meiyan Wang Yue Wang Shouying Huang Yujun Zhao Shengping Wang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Centre of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China

Lignin utilization is a potential approach for replacing fossil energy and releasing the environment ***,we synthesized a series of novel Cu-based catalysts,Cu@NS-SiO_(2)(NS=nano sphere)and alkali metals(Na,K,Rb,and Cs)doped Cu@NS-SiO_(2),and applied them in hydrodeoxygenation reaction of *** Cu dispersion was presented on all *** modification of alkali metals on Cu@NS-SiO_(2) significantly enhanced the electron density of Cu sites in the following order:Cs>Rb>K>Na,among which Cs decreased the Cu_(2)p_(3)/2 binding energy most(by 0.7 eV).Moreover,the modification did not substantially affect the geometric structure of Cu *** regulable electronic environment of Cu sites was crucial for selective deoxygenation and inhibiting the hydrogenation of aromatic rings in anisole,and thus promoted the selectivity of *** with Cu@NS-SiO_(2)(~59%),the highest benzene selectivity was obtained on Cs/10Cu@NS-SiO_(2) at~83%.

关键词： Anisole Hydrodeoxygenation Arenes Alkali metal Electronic effect

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High CO methanation activity on zirconia-supported molybdenum sulfide catalyst

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Journal of Energy Chemistry 2014年第5期23卷 625-632页

作者： Zhenhua Li Ye Tian Jia He Baowei Wang xinbin ma Key Lab for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University

In this study, different methods were used to prepare MoO3/ZrO2 catalysts for sulfur resistant methanation reaction. It was found that MoO3/ZrO2 catalyst prepared by one-step co-precipitation method achieved high methanation performance. CO conversion could reach up to 90% on 25 wt% MoO3/ZrO2 catalyst, much higher than that on the conventional 25 wt% MoO3/Al2O3 catalyst. The Mo-based catalysts were characterized by XRF, XRD, Raman, BET, TEM and H2-TPR etc. It was found that MoO3 particles were highly dispersed on ZrO2 support for 25 wt% MoO3/ZrO2 catalyst prepared at 65-85℃ because of its relatively larger pore size, which contributed to a high CO conversion. Meanwhile, when MoO3 loading exceeded the monolayer coverage, the formed crystalline MoO3 and ZrM020g might block the micropores of the catalyst and make the methanation activity declined. These results are useful for preparing highly efficient catalyst for CO methanation process.

关键词： MoO3/ZrO2 catalyst one-step co-precipitation method sulfur resistant methanation high CO conversion

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Electrocarboxylation of CO_(2) with Organic Substrates:Toward Cathodic Reaction

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Transactions of Tianjin University 2023年第4期29卷 254-274页

作者： He Yao Mei-Yan Wang Chengguang Yue Bangman Feng Wenhao Ji Chunbo Qian Shengping Wang Sheng Zhang xinbin ma School of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of Ministry of EducationCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin 300072China Ningbo Key Laboratory of Green Petrochemical Carbon Emission Reduction Technology and Equipment Zhejiang Institute of Tianjin UniversityNingbo 315200China

Electrocarboxylation of carbon dioxide(CO_(2))using organic substrates has emerged as a promising method for the sustainable synthesis of value-added carboxylic acids due to its renewable energy source and mild reaction *** reactivity and product selectivity of electrocarboxylation are highly dependent on the cathodic behavior,involving a sequence of electron transfers and chemical ***,it is necessary to understand the cathodic reaction mechanisms for optimizing reaction performance and product *** this work,a review of recent advancements in the electrocarboxylation of CO_(2)with organic substrates based on different cathodic reaction pathways is presented to provide a reference for the development of novel methodologies of CO_(2)***,cathodic reactions are particularly classified into two categories based on the initial electron carriers(i.e.,CO_(2)radical anion and substrate radical anion).Furthermore,three cathodic pathways(ENE(N),ENED,and EDEN)of substrate radical anion-induced electrocarboxylation are discussed,which differ in their electron transfer sequence,substrate dissociation,and nucleophilic reaction,to highlight their implications on reactivity and product selectivity.

关键词： Carbon dioxide Electrocatalysis Carboxylation Cathodic reaction Carboxylic acids

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STUDY ON THE CATALYTIC REACTION OF ACETONE TO DIACETONE ALCOHOL

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Chinese Journal of Catalysis 1996年第5期 121-126页

作者： Sun Hongwei, He Fei, Xu Genhui *, ma xinbin (Department of Chemical Engineering, Tianjin University, Tianjin 300072)

ＳＴＵＤＹＯＮＴＨＥＣＡＴＡＬＹＴＩＣＲＥＡＣＴＩＯＮＯＦＡＣＥＴＯＮＥＴＯＤＩＡＣＥＴＯＮＥＡＬＣＯＨＯＬＳｕｎＨｏｎｇｗｅｉ，ＨｅＦｅｉ，ＸｕＧｅｎｈｕｉ＊，ＭａＸｉｎｂｉｎ（ＤｅｐａｒｔｍｅｎｔｏｆＣｈｅｍｉｃ... 详细信息

ＳＴＵＤＹＯＮＴＨＥＣＡＴＡＬＹＴＩＣＲＥＡＣＴＩＯＮＯＦＡＣＥＴＯＮＥＴＯＤＩＡＣＥＴＯＮＥＡＬＣＯＨＯＬＳｕｎＨｏｎｇｗｅｉ，ＨｅＦｅｉ，ＸｕＧｅｎｈｕｉ＊，ＭａＸｉｎｂｉｎ（ＤｅｐａｒｔｍｅｎｔｏｆＣｈｅｍｉｃａｌＥｎｇｉｎｅｒｉｎｇ，Ｔｉａｎ...

关键词： Anion exchange resin Aldol condensation Acetone Diacetone alcohol

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