Interface tuning of Cu+/Cu0 by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst

doi:10.1016/j.jechem.2020.02.038

能源化学(英文版) ›› 2020, Vol. 49 ›› Issue (10): 248-256.DOI: 10.1016/j.jechem.2020.02.038

Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst

Yujun Zhao^a, Huanhuan Zhang^a, Yuxi Xu^a, Shengnian Wang^b, Yan Xu^a, Shengping Wang^a, Xinbin Ma^a

a Key Laboratory for Green Chemical Technology of Ministry of Education,Collaborative Innovation Center of Chemical Science and Engineering,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;
b Chemical Engineering,Institute for Micromanufacturing,Louisiana Tech University,Ruston,LA 71272,USA

收稿日期:2020-01-16 修回日期:2020-02-24 出版日期:2020-10-15 发布日期:2020-12-18
通讯作者: Yujun Zhao
基金资助:
We are grateful to the financial support from the National Natural Science Foundation of China(21878227,U1510203).

Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst

Yujun Zhao^a, Huanhuan Zhang^a, Yuxi Xu^a, Shengnian Wang^b, Yan Xu^a, Shengping Wang^a, Xinbin Ma^a

a Key Laboratory for Green Chemical Technology of Ministry of Education,Collaborative Innovation Center of Chemical Science and Engineering,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;
b Chemical Engineering,Institute for Micromanufacturing,Louisiana Tech University,Ruston,LA 71272,USA

Received:2020-01-16 Revised:2020-02-24 Online:2020-10-15 Published:2020-12-18
Contact: Yujun Zhao
Supported by:
We are grateful to the financial support from the National Natural Science Foundation of China(21878227,U1510203).

摘要/Abstract

摘要： An efficient ZrO₂-doped Cu/SiO₂ catalyst was fabricated through hydrolysis precipitation method (HP) and used to produce ethylene glycol (EG) through dimethyl oxalate (DMO) hydrogenation.The states for zirconia on copper catalyst and roles in DMO hydrogenation were investigated through various characterization tools,including N₂ physical adsorption,XRD,H₂-TPR,Methyl glycolate-TPD-MS,XPS,XAES as well.Compared with common ammonia evaporation and co-precipitation methods used in catalyst preparation,this HP method is found to effectively suppress the agglomeration and further size growth of copper nanoparticles by enhancing the interactions between copper and zirconia species.More importantly,uniform distribution of ZrO₂ dopant is achieved due to the pseudo-homogeneous reactions in the mixing step of catalyst preparation.A proper amount of zirconium dopant helps achieve the desirable proportion of Cu⁺/(Cu⁺+Cu⁰) for surface copper species,especially promotes the production of Cu⁺ species originated from Cu-ZrO₂ species at the interface of copper and zirconia particles.In comparison with Cu⁺ species formed from copper phyllosilicates reduction,the Cu⁺ sites derived from Cu-ZrO₂ species show higher adsorption ability of MG,an important intermediate species in ethylene glycol production.These adsorbed MG molecules further react with atomic hydrogen shifted from adjacent metallic copper surface,leading to a higher catalytic behavior.For the EG production via DMO hydrogenation,the turnover frequency (TOF) normalized by Cu⁰ species on CuZr/SiO₂ catalyst is 1.8 times than that of traditional Cu/SiO₂ counterpart.Due to the enhanced synergy effect between Cu⁺ and Cu⁰ active sites,a lower activation energy of ester hydrogenation on this ZrO₂-doped Cu/SiO₂ catalyst is believed to be responsible for the significant improvement.

关键词: Copper, Zirconia, Hydrogenation, Ethylene glycol

Abstract: An efficient ZrO₂-doped Cu/SiO₂ catalyst was fabricated through hydrolysis precipitation method (HP) and used to produce ethylene glycol (EG) through dimethyl oxalate (DMO) hydrogenation.The states for zirconia on copper catalyst and roles in DMO hydrogenation were investigated through various characterization tools,including N₂ physical adsorption,XRD,H₂-TPR,Methyl glycolate-TPD-MS,XPS,XAES as well.Compared with common ammonia evaporation and co-precipitation methods used in catalyst preparation,this HP method is found to effectively suppress the agglomeration and further size growth of copper nanoparticles by enhancing the interactions between copper and zirconia species.More importantly,uniform distribution of ZrO₂ dopant is achieved due to the pseudo-homogeneous reactions in the mixing step of catalyst preparation.A proper amount of zirconium dopant helps achieve the desirable proportion of Cu⁺/(Cu⁺+Cu⁰) for surface copper species,especially promotes the production of Cu⁺ species originated from Cu-ZrO₂ species at the interface of copper and zirconia particles.In comparison with Cu⁺ species formed from copper phyllosilicates reduction,the Cu⁺ sites derived from Cu-ZrO₂ species show higher adsorption ability of MG,an important intermediate species in ethylene glycol production.These adsorbed MG molecules further react with atomic hydrogen shifted from adjacent metallic copper surface,leading to a higher catalytic behavior.For the EG production via DMO hydrogenation,the turnover frequency (TOF) normalized by Cu⁰ species on CuZr/SiO₂ catalyst is 1.8 times than that of traditional Cu/SiO₂ counterpart.Due to the enhanced synergy effect between Cu⁺ and Cu⁰ active sites,a lower activation energy of ester hydrogenation on this ZrO₂-doped Cu/SiO₂ catalyst is believed to be responsible for the significant improvement.

Key words: Copper, Zirconia, Hydrogenation, Ethylene glycol

Yujun Zhao, Huanhuan Zhang, Yuxi Xu, Shengnian Wang, Yan Xu, Shengping Wang, Xinbin Ma. Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst[J]. 能源化学(英文版), 2020, 49(10): 248-256.

参考文献

[1] J.Ding,T.Popa,J.K.Tang,K.A.M.Gasem,M.H.Fan,Q.Zhong,Appl.Catal.B 209(2017)530-542.
[2] L.Li,D.Z.Ren,J.Fu,Y.J.Liu,F.M.Jin,Z.B.Huo,J.Energy Chem.25(2016)507-511.
[3] A.Y.Yin,J.W.Qu,X.Y.Guo,W.L.Dai,K.N.Fan,Appl.Catal.A 400(2011)39-47.
[4] R.P.Ye,L.Lin,J.X.Yang,M.L.Sun,F.Li,B.Li,Y.G.Yao,J.Catal.350(2017)122-132.
[5] J.Sun,J.F.Yu,Q.X.Ma,F.Q.Meng,X.X.Wei,Y.N.Sun,N.Tsubaki,Sci.Adv.4(2018).
[6] Y.J.Zhao,S.Zhao,Y.C.Geng,Y.L.Shen,H.R.Yue,J.Lv,S.P.Wang,X.B.Ma,Catal.Today 276(2016)28-35.
[7] J.Wu,G.Gao,Y.Li,P.Sun,J.Wang,F.W.Li,Appl.Catal.B 245(2019)251-261.
[8] Y.Sun,F.Meng,Q.Ge,J.Sun,ChemistryOpen 7(2018)969-976.
[9] Z.He,H.Q.Lin,P.He,Y.Z.Yuan,J.Catal.277(2011)54-63.
[10] P.P.Ai,M.H.Tan,P.Reubroycharoen,Y.Wang,X.B.Feng,G.G.Liu,G.H.Yang,N.Tsubaki,Catal.Sci.Technol.8(2018)6441-6451.
[11] H.B.Yu,W.Q.Tang,K.J.Li,H.F.Yin,S.L.Zhao,S.H.Zhou,Chem.Eng.Sci.196(2019)402-413.
[12] M.M.Li,J.Zheng,J.Qu,F.Liao,E.Raine,W.C.Kuo,S.S.Su,P.Po,Y.Yuan,S.C.Tsang,Sci.Rep.6(2016)20527.
[13] L.He,X.X.Gong,L.M.Ye,X.P.Duan,Y.Z.Yuan,J.Energy Chem.25(2016)1038-1044.
[14] X.L.Zheng,H.Q.Lin,J.W.Zheng,X.P.Duan,Y.Z.Yuan,ACS Catal.3(2013)2738-2749.
[15] J.Wu,G.Gao,P.Sun,X.D.Long,F.W.Li,ACS Catal.7(2017)7890-7901.
[16] X.B.Yu,T.A.Vest,N.Gleason-Boure,S.G.Karakalos,G.L.Tate,M.Burkholder,J.R.Monnier,C.T.Williams,J.Catal.380(2019)289-296.
[17] T.Kondratowicz,M.Drozdek,A.Rokicińska,P.Natkański,M.Michalik,P.Kuśtrowski,Microporous Mesoporous Mater.279(2019)446-455.
[18] Y.F.Zhu,X.Kong,H.Y.Zheng,Y.L.Zhu,Mol.Catal.458(2018)73-82.
[19] I.U.Din,M.S.Shaharun,A.Naeem,S.Tasleem,P.Ahmad,J.Energy Chem.39(2019)68-76.
[20] J.Schittkowski,K.Tölle,S.Anke,S.Stürmer,M.Muhler,J.Catal.352(2017)120-129.
[21] A.G.Sato,D.P.Volanti,D.M.Meira,S.Damyanova,E.Longo,J.M.C.Bueno,J.Catal.307(2013)1-17.
[22] Y.Wang,S.Kattel,W.Gao,K.Li,P.Liu,J.G.Chen,H.Wang,Nat.Commun.10(2019)1166.
[23] F.L.Deng,N.Li,S.Y.Tang,C.J.Liu,H.R.Yue,B.Liang,Chem.Eng.J.334(2018)1943-1953.
[24] S.L.Li,Y.F.Zan,Y.Y.Sun,Z.C.Tan,G.Miao,L.Z.Kong,Y.H.Sun,J.Energy Chem.28(2019)101-106.
[25] I.Orlowski,M.Douthwaite,S.Iqbal,J.S.Hayward,T.E.Davies,J.K.Bartley,P.J.Miedziak,J.Hirayama,D.J.Morgan,D.J.Willock,G.J.Hutchings,J.Energy Chem.36(2019)15-24.
[26] E.Lam,K.Larmier,P.Wolf,S.Tada,O.V.Safonova,C.Coperet,J.Am.Chem.Soc.140(2018)10530-10535.
[27] S.Tada,S.Kayamori,T.Honma,H.Kamei,A.Nariyuki,K.Kon,T.Toyao,K.Shimizu,S.Satokawa,ACS Catal.8(2018)7809-7819.
[28] S.Zhao,H.R.Yue,Y.J.Zhao,B.Wang,Y.C.Geng,J.Lv,S.P.Wang,J.L.Gong,X.B.Ma,J.Catal.297(2013)142-150.
[29] J.L.Gong,H.R.Yue,Y.J.Zhao,S.Zhao,L.Zhao,J.Lv,S.P.Wang,X.B.Ma,J.Am.Chem.Soc.134(2012)13922-13925.
[30] Y.J.Zhao,B.Shan,Y.Wang,J.H.Zhou,S.P.Wang,X.B.Ma,Ind.Eng.Chem.Res.57(2018)4526-4534.
[31] Y.J.Zhao,S.M.Li,Y.Wang,B.Shan,J.Zhang,S.P.Wang,X.B.Ma,Chem.Eng.J.313(2017)759-768.
[32] P.F.Ma,Z.H.Xiao,S.H.Jin,C.Li,C.H.Liang,J.Energy Chem.25(2016)782-792.
[33] Y.F.Zhu,Y.L.Zhu,G.Q.Ding,S.H.Zhu,H.Y.Zheng,Y.W.Li,Appl.Catal.A 468(2013)296-304.
[34] W.L.Yang,Y.J.Zhao,S.P.Wang,X.B.Ma,Chem.Ind.Eng.33(2016)1-5.
[35] C.J.Yang,Z.L.Miao,F.Zhang,L.Li,Y.T.Liu,A.Q.Wang,T.Zhang,Green Chem.20(2018)2142-2150.
[36] F.Li,C.S.Lu,X.N.Li,Chin.Chem.Lett.25(2014)1461-1465.
[37] Q.Wang,L.Qiu,D.Ding,Y.Z.Chen,C.W.Shi,P.Cui,Y.Wang,Q.H.Zhang,R.Liu,H.Shen,Catal.Commun.108(2018)68-72.
[38] K.A.Resende,C.A.Teles,G.Jacobs,B.H.Davis,D.C.Cronauer,A.Jeremy Kropf,C.L.Marshall,C.E.Hori,F.B.Noronha,Appl.Catal.B 232(2018)213-231.
[39] S.M.Li,Y.Wang,J.Zhang,S.P.Wang,Y.Xu,Y.J.Zhao,X.B.Ma,Ind.Eng.Chem.Res.54(2015)1243-1250.
[40] K.Z.Li,J.G.Chen,ACS Catal.9(2019)7840-7861.
[41] R.P.Ye,L.Lin,C.C.Chen,J.X.Yang,F.Li,X.Zhang,D.J.Li,Y.Y.Qin,Z.F.Zhou,Y.G.Yao,ACS Catal.8(2018)3382-3394.
[42] Y.F.Zhu,X.Kong,D.B.Cao,J.L.Cui,Y.L.Zhu,Y.W.Li,ACS Catal.4(2014)3675-3681.
[43] P.P.Ai,M.H.Tan,N.Yamane,G.G.Liu,R.G.Fan,G.H.Yang,Y.Yoneyama,R.Q.Yang,N.Tsubaki,Chemistry(Easton)23(2017)8252-8261.
[44] X.X.Gong,M.L.Wang,H.H.Fang,X.Q.Qian,L.M.Ye,X.P.Duan,Y.Z.Yuan,Chem.Commun.(Camb)53(2017)6933-6936.
[45] H.R.Yue,Y.J.Zhao,S.Zhao,B.Wang,X.B.Ma,J.L.Gong,Nat Commun.4(2013)2339.
[46] Z.Q.Wang,Z.N.Xu,S.Y.Peng,M.J.Zhang,G.Lu,Q.S.Chen,Y.M.Chen,G.C.Guo,ACS Catal.5(2015)4255-4259.
[47] Y.B.Song,J.Zhang,J.Lv,Y.J.Zhao,X.B.Ma,Ind.Eng.Chem.Res.54(2015)9699-9707.
[48] Q.L.Tang,Q.J.Hong,Z.P.Liu,J.Catal.263(2009)114-122.
[49] D.Kim,J.Resasco,Y.Yu,A.M.Asiri,P.Yang,Nat.Commun.5(2014)4948.

Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst

Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst

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