Cerium coordination-dependent surface intermediates regulate activity in dimethyl carbonate synthesis from CO2 and methanol
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作者:
Tian, Linyuan
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City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R ChinaCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Tian, Linyuan
[1
]
Tan, Zicong
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City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R ChinaCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Tan, Zicong
[1
]
Wang, Quan
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City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R ChinaCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Wang, Quan
[1
]
Liao, Yin -Song
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机构:
Natl Tsing Hua Univ, Dept Mat Sci & Engn, Hsinchu 300, TaiwanCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Liao, Yin -Song
[2
]
Chou, Jyh-Pin
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Natl Changhua Univ Educ, Dept & Grad Inst Phys, Changhua 500, TaiwanCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Chou, Jyh-Pin
[3
]
Wu, Jyh-Ming
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Natl Tsing Hua Univ, Dept Mat Sci & Engn, Hsinchu 300, TaiwanCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Wu, Jyh-Ming
[2
]
Liu, Guoliang
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Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R ChinaCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Liu, Guoliang
[4
]
Peng, Yung-Kang
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City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
City Univ Hong Kong, Shenzhen Res Inst, Shenzhen 518057, Peoples R ChinaCity Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
Peng, Yung-Kang
[1
,5
]
机构:
[1] City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
The direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol is a potential green alternative to the current industrial methods using toxic chemicals. Although many CeO2-based catalysts have been explored, the key structural factor affecting their DMC activity is still unclear. Herein, single-crystalline CeO2 catalysts bearing distinct but well-defined Ce coordination structures were examined. We found that methanol is the key species being activated by surface Ce sites (cf. CO2) to produce methyl carbonate (MC) and later DMC. The reactivity of surface methoxy species towards CO2 varies considerably with its configuration determined by Ce coordination structures. The head-to-head terminal methoxy species converts CO2 to MC faster than its atilt counterparts, resulting in a higher DMC activity. The bridging methoxy species is, however, too stable to react with CO2. The established structure-activity relation here should also guide the design of CeO2-based catalysts in other reactions involving methanol activation.
机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Fu, Zhongwei
Zhong, Yunyun
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Zhong, Yunyun
Yu, Yuehong
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Yu, Yuehong
Long, Lizhen
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Long, Lizhen
Xiao, Min
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Xiao, Min
Han, Dongmei
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Han, Dongmei
Wang, Shuanjin
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Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R ChinaSun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Wang, Shuanjin
Meng, Yuezhong
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Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R ChinaSun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Fu, Zhongwei
Zhong, Yunyun
论文数: 0引用数: 0
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Zhong, Yunyun
Yu, Yuehong
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Yu, Yuehong
Long, Lizhen
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Long, Lizhen
Xiao, Min
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机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Xiao, Min
Han, Dongmei
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h-index: 0
机构:Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Han, Dongmei
Wang, Shuanjin
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机构:
Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R ChinaSun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China
Wang, Shuanjin
Meng, Yuezhong
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机构:
Sun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R ChinaSun Yat Sen Univ, Key Lab Low Carbon Chem & Energy Conservat Guangd, 135 Xingang Xi Rd, Guangzhou 510275, Guangdong, Peoples R China