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Role of Re and Ru in Re-Ru/C Bimetallic Catalysts for the Aqueous Hydrogenation of Succinic Acid
Di, Xin; Li, Chuang; Zhang, Bingsen; Qi, Ji; Li, Wenzhen; Su, Dangsheng; Liang, Changhai; Liang, CH (reprint author), Dalian Univ Technol, Sch Chem Engn, Lab Adv Mat & Catalyt Engn, Dalian 116024, Peoples R China.
2017-04-26
发表期刊INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
ISSN0888-5885
卷号56期号:16页码:4672-4683
摘要To obtain an effective supported metallic catalyst for aqueous hydrogenation of succinic acid (SA), C-supported Re-Ru catalysts with different Re/Ru ratios were sought by using a convenient and environmentally friendly microwave-assisted thermolytic method. The results indicate that the as-prepared Re-Ru/C catalysts exhibit high dispersion with fairly small average particle size (0.7-1.6 nm) and well structural properties. During the transformation of SA, the Ru composition is responsible for the hydrogenolysis of SA, while the Re composition favors the hydrogenation of SA. The bimetallic Re Ru interaction promotes the formation of 1,4-butanediol (selectivity is 70.1% with complete conversion), which could rarely be detected when using Re/C or Ru/C monometallic catalysts. The kinetic study further reveals that the introduction of Ru significantly reduces the apparent activation energy from 62 to 40 kJ mol(-1) and increases the saturation ability of hydrogenation intermediates on the surface of catalysts compared with Re/C. A Re Ru/C bimetallic catalyst accelerates the formation rate of 1,4-butanediol relative to that of tetrahydrofuran. According to a kinetic mechanism, ring opening of gamma-butyrolactone is favored at low temperature, while direct hydrogenation is favored at high temperature:; To obtain an effective supported metallic catalyst for aqueous hydrogenation of succinic acid (SA), C-supported Re-Ru catalysts with different Re/Ru ratios were sought by using a convenient and environmentally friendly microwave-assisted thermolytic method. The results indicate that the as-prepared Re-Ru/C catalysts exhibit high dispersion with fairly small average particle size (0.7-1.6 nm) and well structural properties. During the transformation of SA, the Ru composition is responsible for the hydrogenolysis of SA, while the Re composition favors the hydrogenation of SA. The bimetallic Re Ru interaction promotes the formation of 1,4-butanediol (selectivity is 70.1% with complete conversion), which could rarely be detected when using Re/C or Ru/C monometallic catalysts. The kinetic study further reveals that the introduction of Ru significantly reduces the apparent activation energy from 62 to 40 kJ mol(-1) and increases the saturation ability of hydrogenation intermediates on the surface of catalysts compared with Re/C. A Re Ru/C bimetallic catalyst accelerates the formation rate of 1,4-butanediol relative to that of tetrahydrofuran. According to a kinetic mechanism, ring opening of gamma-butyrolactone is favored at low temperature, while direct hydrogenation is favored at high temperature:
部门归属[di, xin ; li, chuang ; qi, ji ; liang, changhai] dalian univ technol, sch chem engn, lab adv mat & catalyt engn, dalian 116024, peoples r china ; [zhang, bingsen ; su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china ; [li, wenzhen] iowa state univ, dcbe, biorenewables res lab, ames, ia 50011 usa
学科领域Engineering, Chemical
资助者National Natural Science Foundation of China [21573031, 21428301]; Fundamental Research Funds for the Central Universities [DUT15ZD106]; Program for Excellent Talents in Dalian City [2016RD09]
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/78176
专题中国科学院金属研究所
通讯作者Liang, CH (reprint author), Dalian Univ Technol, Sch Chem Engn, Lab Adv Mat & Catalyt Engn, Dalian 116024, Peoples R China.
推荐引用方式
GB/T 7714
Di, Xin,Li, Chuang,Zhang, Bingsen,et al. Role of Re and Ru in Re-Ru/C Bimetallic Catalysts for the Aqueous Hydrogenation of Succinic Acid[J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH,2017,56(16):4672-4683.
APA Di, Xin.,Li, Chuang.,Zhang, Bingsen.,Qi, Ji.,Li, Wenzhen.,...&Liang, CH .(2017).Role of Re and Ru in Re-Ru/C Bimetallic Catalysts for the Aqueous Hydrogenation of Succinic Acid.INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH,56(16),4672-4683.
MLA Di, Xin,et al."Role of Re and Ru in Re-Ru/C Bimetallic Catalysts for the Aqueous Hydrogenation of Succinic Acid".INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 56.16(2017):4672-4683.
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