Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol
Li, Fengjiao1,2; Wang, Liguo1; Han, Xiao1; He, Peng1; Cao, Yan1; Li, Huiquan1
2016
发表期刊RSC ADVANCES
ISSN2046-2069
卷号6期号:51页码:45894-45906
摘要Hydrogenation of ethylene carbonate (EC) is an attractive and promising approach for indirect hydrogenation of CO2 to co-produce ethylene glycol (EG) and methanol (MeOH). In this work, thermodynamics of EC hydrogenation was firstly calculated, and the results disclosed that EC hydrogenation is exothermic (Delta H-r(m)theta = -71.59 kJ mol(-1)) and thermodynamically favorable (Delta(r)G(m)(theta) = -25.62 kJ mol(-1)). The mesoporous silica supported copper catalysts were successfully prepared by facile ammonia evaporation method using KIT-6, MCM-41 and SBA-15 as support materials. The asprepared Cu/KIT-6, Cu/MCM-41 and Cu/SBA-15 were thoroughly characterized by N-2 physisorption, ICP-AES, N2O titration, FT-IR, XRD, H-2-TPR, TEM, XPS and XAES. It was found that copper nanoparticles were well dispersed on these supports. Interestingly, a larger metallic Cu surface area with higher dispersion was obtained on SBA-15 when compared with KIT-6 and MCM-41. Furthermore, Cu-0 and Cu+ species in various ratios were verified to co-exist on the surfaces of the three catalysts, which originated from CuO and copper phyllosilicate, respectively. The catalytic performances showed that Cu/SBA-15 exhibited a superior catalytic activity with a TON of 22.0 and 11.4 (mol mol(-1)) towards EG and MeOH, respectively. Importantly, 100% of EC conversion, 94.7% of EG yield and 62.3% of MeOH yield were achieved within a short reaction time of 4 h over Cu/SBA-15 under optimized conditions. The synergetic effect between Cu-0 and Cu+ species, in which it was proposed that Cu-0 species dissociated H-2, while Cu+ species absorbed the carbonyl group of EC, was responsible for the higher catalytic activity of Cu/SBA-15.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1039/c6ra06464g
收录类别SCI
语种英语
关键词[WOS]DIMETHYL OXALATE ; MESOPOROUS SILICA ; CYCLIC CARBONATES ; CU/SIO2 CATALYSTS ; SBA-15 ; COPOLYMER ; TRIBLOCK ; DIOXIDE ; HYDROGENOLYSIS ; EFFICIENT
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
项目资助者National Natural Science Foundation of China(21576272 ; National Key Technology RD Program(2013BAC11B03) ; 21406245)
WOS记录号WOS:000376120100110
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/21078
专题湿法冶金清洁生产技术国家工程实验室
作者单位1.Chinese Acad Sci, Inst Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Li, Fengjiao,Wang, Liguo,Han, Xiao,et al. Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol[J]. RSC ADVANCES,2016,6(51):45894-45906.
APA Li, Fengjiao,Wang, Liguo,Han, Xiao,He, Peng,Cao, Yan,&Li, Huiquan.(2016).Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol.RSC ADVANCES,6(51),45894-45906.
MLA Li, Fengjiao,et al."Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol".RSC ADVANCES 6.51(2016):45894-45906.
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