Chem. J. Chinese Universities ›› 2022, Vol. 43 ›› Issue (6): 20210842.doi: 10.7503/cjcu20210842
• Physical Chemistry • Previous Articles Next Articles
SONG Youwei, AN Jiangwei, WANG Zheng, WANG Xuhui, QUAN Yanhong, REN Jun, ZHAO Jinxian()
Received:
2021-12-20
Online:
2022-06-10
Published:
2022-04-04
Contact:
ZHAO Jinxian
E-mail:zhaojinxian@tyut.edu.cn
Supported by:
CLC Number:
TrendMD:
SONG Youwei, AN Jiangwei, WANG Zheng, WANG Xuhui, QUAN Yanhong, REN Jun, ZHAO Jinxian. Effects of Ag,Zn,Pd-doping on Catalytic Performance of Copper Catalyst for Selective Hydrogenation of Dimethyl Oxalate[J]. Chem. J. Chinese Universities, 2022, 43(6): 20210842.
Species | Cu(111)[ | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | ||||
---|---|---|---|---|---|---|---|---|
Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | |
H2 | Fcc | 13.3 | Fcc | 40.4 | Fcc | 44.6 | Fcc | 26.3 |
H | Fcc | 247.6 | Fcc | 236.7 | Fcc | 229.6 | Fcc | 253.3 |
DMO | — | 46 | — | 55.1 | — | 50.1 | — | 57.8 |
CH3OOCCO | Top | 152 | Top | 151.1 | Top | 151.4 | Top | 199.6 |
CH3O | Hcp | 222 | Fcc | 206.2 | Hcp | 221.2 | Fcc | 203.5 |
CH3OOCCOH | Top(C) Bridge(O) | 48 | Top(C) Top(O) | 301 | Bridge(C) Top(O) | 301 | Top(C) Top(O) | 327.7 |
CH3OOCCHOH | Top(C) Top(O) | 101.5 | Top | 96.5 | Top | 129 | Top | 146.6 |
MG | — | 56.1 | — | 50.4 | — | 35.4 | — | 38.2 |
CH3OH | — | 36.7 | — | 41.5 | — | 43.1 | — | 43.3 |
OCCH2OH | Top | 177.3 | Top | 172.4 | Top | 168.7 | Top | 220.6 |
Table 1 Adsorption sites and adsorption energies of all species involved in DMO hydrogenation to MG on Cu(111), Ag-Cu(111), Zn-Cu(111) and Pd-Cu(111) surfaces
Species | Cu(111)[ | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | ||||
---|---|---|---|---|---|---|---|---|
Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | |
H2 | Fcc | 13.3 | Fcc | 40.4 | Fcc | 44.6 | Fcc | 26.3 |
H | Fcc | 247.6 | Fcc | 236.7 | Fcc | 229.6 | Fcc | 253.3 |
DMO | — | 46 | — | 55.1 | — | 50.1 | — | 57.8 |
CH3OOCCO | Top | 152 | Top | 151.1 | Top | 151.4 | Top | 199.6 |
CH3O | Hcp | 222 | Fcc | 206.2 | Hcp | 221.2 | Fcc | 203.5 |
CH3OOCCOH | Top(C) Bridge(O) | 48 | Top(C) Top(O) | 301 | Bridge(C) Top(O) | 301 | Top(C) Top(O) | 327.7 |
CH3OOCCHOH | Top(C) Top(O) | 101.5 | Top | 96.5 | Top | 129 | Top | 146.6 |
MG | — | 56.1 | — | 50.4 | — | 35.4 | — | 38.2 |
CH3OH | — | 36.7 | — | 41.5 | — | 43.1 | — | 43.3 |
OCCH2OH | Top | 177.3 | Top | 172.4 | Top | 168.7 | Top | 220.6 |
Elementary step | Reaction |
---|---|
R1 | H2+2*?2H* |
R2 | CH3OOCCOOCH3 + 2*→CH3OOCC*O + CH3O* |
R3 | CH3OOCC*O + H*?CH3OOCC*OH(CH3OOCC*HO)+ * |
R4 | CH3OOCC*OH(CH3OOCC*HO) + H*? CH3OOCC*HOH + * |
R5 | CH3OOCC*HOH + H*? CH3OOCC*H2OH + * |
R6 | CH3O* + H*? CH3OH* + * |
R7 | CH3OOCCH2OH+2*?HOCH2C*O+CH3O* |
Table 2 Mechanism of DMO hydrogenation over Cu catalyst#
Elementary step | Reaction |
---|---|
R1 | H2+2*?2H* |
R2 | CH3OOCCOOCH3 + 2*→CH3OOCC*O + CH3O* |
R3 | CH3OOCC*O + H*?CH3OOCC*OH(CH3OOCC*HO)+ * |
R4 | CH3OOCC*OH(CH3OOCC*HO) + H*? CH3OOCC*HOH + * |
R5 | CH3OOCC*HOH + H*? CH3OOCC*H2OH + * |
R6 | CH3O* + H*? CH3OH* + * |
R7 | CH3OOCCH2OH+2*?HOCH2C*O+CH3O* |
Elementary step | Cu(111)[ | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | |||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | |
R1 | — | -13.3 | — | — | -40.4 | — | — | -44.6 | — | — | -26.3 |
R2 | 220.2 | 86.2 | TS1 | 224.3 | 91.6 | TS5 | 158.5 | 75.6 | TS9 | 327.2 | 39.7 |
R3 | 60.1 | -39.8 | TS2 | 68.5 | -19.9 | TS6 | 115.1 | -10.3 | TS10 | 134.7 | 2.5 |
R4 | 23.7 | -38.2 | TS3 | 74.6 | -75 | TS7 | 91.9 | -89.9 | TS11 | 58.2 | -90.7 |
R5 | 91.5 | -73.3 | TS4 | 47.3 | -107 | TS8 | 104.2 | -58.3 | TS12 | 171.5 | -35.1 |
R6 | 111.3 | -20.3 | TS13 | 141.7 | -39.8 | TS14 | 138.9 | -43.1 | TS15 | 141.3 | -36.1 |
R7 | 192.6 | 88.4 | TS16 | 321.4 | 101 | TS17 | 305.9 | 68.9 | TS18 | 75.6 | 40 |
Table 3 Activation energies(Ea) and reaction energies(ΔH) for elementary reactions(R1—R5) of DMO hydrogenation to MG and side reactions(R6, R7) on Cu(111) and M-Cu(111) surfaces
Elementary step | Cu(111)[ | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | |||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | |
R1 | — | -13.3 | — | — | -40.4 | — | — | -44.6 | — | — | -26.3 |
R2 | 220.2 | 86.2 | TS1 | 224.3 | 91.6 | TS5 | 158.5 | 75.6 | TS9 | 327.2 | 39.7 |
R3 | 60.1 | -39.8 | TS2 | 68.5 | -19.9 | TS6 | 115.1 | -10.3 | TS10 | 134.7 | 2.5 |
R4 | 23.7 | -38.2 | TS3 | 74.6 | -75 | TS7 | 91.9 | -89.9 | TS11 | 58.2 | -90.7 |
R5 | 91.5 | -73.3 | TS4 | 47.3 | -107 | TS8 | 104.2 | -58.3 | TS12 | 171.5 | -35.1 |
R6 | 111.3 | -20.3 | TS13 | 141.7 | -39.8 | TS14 | 138.9 | -43.1 | TS15 | 141.3 | -36.1 |
R7 | 192.6 | 88.4 | TS16 | 321.4 | 101 | TS17 | 305.9 | 68.9 | TS18 | 75.6 | 40 |
Species | Cu2O(111)[ | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | ||||
---|---|---|---|---|---|---|---|---|
Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | |
H2 | Cucus | 31.7 | Cucus | 29.1 | Cucus | 77.6 | Cucus | 32.3 |
H | Osuf | 231.1 | Cucus | 276.1 | Cucus | 265.0 | Bridge (Cucus?Cucsa) | 255.1 |
DMO | Cucus | 101.3 | Cucus | 98.4 | Cucus | 98.6 | Cucus | 100.0 |
CH3OOCCO | Cucus | 200.7 | Cucus | 226.2 | Cucus | 242.6 | Cucus | 246.6 |
CH3O | Cucus | 231.1 | Cucus | 277.1 | Cucus | 242.4 | Cucus | 250.0 |
CH3OOCCHO | Cucus | 88.3 | Cucus | 126.2 | Cucus | 117.6 | Cucus | 151.6 |
CH3OOCCHOH | Cucus | 140.4 | Cucus | 198.5 | Cucus | 175.8 | Cucus | 181.8 |
MG | Cucus | 107.1 | Cucus | 111.0 | Cucus | 121.3 | Cucus | 129.4 |
CH3OH | Cucus | 97.2 | Cucus | 86.3 | Cucus | 110.1 | Cucus | 98.1 |
OCCH2OH | Cucus | 323.1 | Cucus | 267.0 | Cucus | 250.9 | Cucus | 232.3 |
Table 4 Adsorption sites and adsorption energies(Eads) of all species involved in DMO hydrogenation to MG on Cu2O(111) and M?Cu2O(111) surfaces
Species | Cu2O(111)[ | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | ||||
---|---|---|---|---|---|---|---|---|
Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | Site | Eads/(kJ?mol-1) | |
H2 | Cucus | 31.7 | Cucus | 29.1 | Cucus | 77.6 | Cucus | 32.3 |
H | Osuf | 231.1 | Cucus | 276.1 | Cucus | 265.0 | Bridge (Cucus?Cucsa) | 255.1 |
DMO | Cucus | 101.3 | Cucus | 98.4 | Cucus | 98.6 | Cucus | 100.0 |
CH3OOCCO | Cucus | 200.7 | Cucus | 226.2 | Cucus | 242.6 | Cucus | 246.6 |
CH3O | Cucus | 231.1 | Cucus | 277.1 | Cucus | 242.4 | Cucus | 250.0 |
CH3OOCCHO | Cucus | 88.3 | Cucus | 126.2 | Cucus | 117.6 | Cucus | 151.6 |
CH3OOCCHOH | Cucus | 140.4 | Cucus | 198.5 | Cucus | 175.8 | Cucus | 181.8 |
MG | Cucus | 107.1 | Cucus | 111.0 | Cucus | 121.3 | Cucus | 129.4 |
CH3OH | Cucus | 97.2 | Cucus | 86.3 | Cucus | 110.1 | Cucus | 98.1 |
OCCH2OH | Cucus | 323.1 | Cucus | 267.0 | Cucus | 250.9 | Cucus | 232.3 |
Elementary step | Cu2O(111)[ | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | |||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | |
R1 | 299 | -15.1 | TS37 | 66.3 | -9.1 | — | — | -77.6 | TS38 | 57.6 | -9.8 |
R2 | 140.5 | 139.8 | TS19 | 178.9 | 121.7 | TS23 | 187.4 | 105.6 | TS27 | 203.5 | 137.6 |
R3 | 99.2 | 5.1 | TS20 | 65.1 | -61.7 | TS24 | 83.7 | -71.6 | TS28 | 106.4 | -116.3 |
R4 | 68.2 | -16.5 | TS21 | 66.9 | -72.1 | TS25 | 52.6 | -93.8 | TS29 | 87.9 | -15 |
R5 | 244 | -190.7 | TS22 | 32.5 | -77.8 | TS26 | 82.7 | -40.7 | TS30 | 52.7 | -91.9 |
R6 | 6.7 | -53.1 | TS31 | 73.6 | -76.7 | TS32 | 83.8 | -88.4 | TS33 | 31.5 | -73.3 |
R7 | 229 | 147.3 | TS34 | 316 | -12.1 | TS35 | 306.6 | 11.1 | TS36 | 138.7 | 74.6 |
Table 5 Activation energies(Ea) and reaction energies(ΔH) for elementary reactions(R1—R5) of DMO hydrogenation to MG and side reactions(R6, R7) on Cu2O(111) and M-Cu2O(111) surfaces
Elementary step | Cu2O(111)[ | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | |||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | TS | Ea/ (kJ?mol-1) | ΔH/ (kJ?mol-1) | |
R1 | 299 | -15.1 | TS37 | 66.3 | -9.1 | — | — | -77.6 | TS38 | 57.6 | -9.8 |
R2 | 140.5 | 139.8 | TS19 | 178.9 | 121.7 | TS23 | 187.4 | 105.6 | TS27 | 203.5 | 137.6 |
R3 | 99.2 | 5.1 | TS20 | 65.1 | -61.7 | TS24 | 83.7 | -71.6 | TS28 | 106.4 | -116.3 |
R4 | 68.2 | -16.5 | TS21 | 66.9 | -72.1 | TS25 | 52.6 | -93.8 | TS29 | 87.9 | -15 |
R5 | 244 | -190.7 | TS22 | 32.5 | -77.8 | TS26 | 82.7 | -40.7 | TS30 | 52.7 | -91.9 |
R6 | 6.7 | -53.1 | TS31 | 73.6 | -76.7 | TS32 | 83.8 | -88.4 | TS33 | 31.5 | -73.3 |
R7 | 229 | 147.3 | TS34 | 316 | -12.1 | TS35 | 306.6 | 11.1 | TS36 | 138.7 | 74.6 |
Species | Charge transfer, Q/|e| | |||
---|---|---|---|---|
Cu(111) | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | |
DMO | 0.0194 | -0.0942 | 0.0038 | 0.1498 |
MG | -0.0630 | -0.0851 | -0.0702 | -0.0283 |
Table 6 Charge transfer(Q) between DMO, MG and Cu(111), Ag?Cu(111) and Zn?Cu(111) catalysts
Species | Charge transfer, Q/|e| | |||
---|---|---|---|---|
Cu(111) | Ag?Cu(111) | Zn?Cu(111) | Pd?Cu(111) | |
DMO | 0.0194 | -0.0942 | 0.0038 | 0.1498 |
MG | -0.0630 | -0.0851 | -0.0702 | -0.0283 |
Species | Charge transfer, Q/|e| | |||
---|---|---|---|---|
Cu2O(111) | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | |
DMO | 0.0934 | 0.0917 | 0.0913 | 0.1507 |
MG | 0.0129 | 0.0048 | -0.0047 | -0.0002 |
Table 7 Charge transfer(Q) between DMO, MG and Cu2O(111), Ag-Cu2O(111) and Zn?Cu2O(111) catalysts
Species | Charge transfer, Q/|e| | |||
---|---|---|---|---|
Cu2O(111) | Ag?Cu2O(111) | Zn?Cu2O(111) | Pd?Cu2O(111) | |
DMO | 0.0934 | 0.0917 | 0.0913 | 0.1507 |
MG | 0.0129 | 0.0048 | -0.0047 | -0.0002 |
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