Performance of Cu-BTC-derived CuO<sub>x</sub>/C for methanol oxidative carbonylation to dimethyl carbonate

LI Wenjie; GAO Shanlin; LAI Chunbo; XIAO Wanjing; LI Xinling; LIN Huibo; WANG Xinyu; XU Chenghua; DEN Zhiyong

Volume 41 Issue 7

Jul. 2024

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Article Navigation > Acta Materiae Compositae Sinica > 2024 > 41(7): 3624-3633

LI Wenjie, GAO Shanlin, LAI Chunbo, et al. Performance of Cu-BTC-derived CuOx/C for methanol oxidative carbonylation to dimethyl carbonate[J]. Acta Materiae Compositae Sinica, 2024, 41(7): 3624-3633.

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LI Wenjie, GAO Shanlin, LAI Chunbo, et al. Performance of Cu-BTC-derived CuO_x/C for methanol oxidative carbonylation to dimethyl carbonate[J]. Acta Materiae Compositae Sinica, 2024, 41(7): 3624-3633.

LI Wenjie, GAO Shanlin, LAI Chunbo, et al. Performance of Cu-BTC-derived CuOx/C for methanol oxidative carbonylation to dimethyl carbonate[J]. Acta Materiae Compositae Sinica, 2024, 41(7): 3624-3633.

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Performance of Cu-BTC-derived CuO_x/C for methanol oxidative carbonylation to dimethyl carbonate

1.
Air Environmental Modeling and Pollution Controlling Key Laboratory of Sichuan Higher Education Institutes, China-Serbia “the Belt and Road” Joint Laboratory on Environment and Energy, College of Resources and Environment, Chengdu University of Information Technology (CUIT), Chengdu 610225
2.
Shanghai Engineering Research Center of Coal-based Polygeneration, Shanghai Huayi Holding Group Co., Ltd, Shanghai 200040

Funds: Supported by Sichuan Science and Technology Program (Grant No. 2022ZYD0049 and 2021YFG0225), Foundation of Shanghai Engineering Research Center of Coal-based Polygeneration (No. GZKF-MJDLC-03) and Scientific Research Foundation of Chengdu University of Information Technology (Grant No. KYTZ202118).

Received Date: 2023-09-18
Accepted Date: 2023-11-23
Rev Recd Date: 2023-11-05

Available Online: 2023-12-12

Publish Date: 2024-07-15

Abstract

Abstract

Carbon-based material supported Cu is an efficient catalyst for methanol oxidative carbonylation to dimethyl carbonate, but Cu nanoparticles are prone to agglomeration and oxidation. Cu-BTC were prepared by hydrothermal method. And then CuO_x/C catalysts was prepared by pyrolysis Cu-BTC under N₂ atmosphere. The effect of pyrolysis temperature on Cu nanoparticle size, Cu valence state and performance for methanol oxidative carbonylation to dimethyl carbonate were investigated. The characterization results show that increasing the pyrolysis temperature is beneficial to the reduction of Cu²⁺ to (Cu⁰+Cu⁺), but would lead to the agglomeration of Cu nanoparticles. Catalytic activity decreases with the increasing of pyrolysis temperature. CuO_x/C-300, prepared by pyrolysis of Cu-BTC at 300 ℃, shows the optimized catalytic activity and the space-time yield of dimethyl carbonate is 1209 mg·g⁻¹·h⁻¹. This is attributed to the smallest particle size of Cu nanoparticles (7.5 nm). In addition, the space-time yield of dimethyl carbonate decreased to 468 mg·g⁻¹·h⁻¹ after 6 cycle experiments. The main reasons for catalyst inactivation are the oxidation of (Cu⁰+Cu⁺) and the agglomeration of Cu nanoparticles.
- catalyst,
- carbon-based materials,
- Cu nanoparticles,
- dimethyl carbonate,
- MOFs,
- pyrolysis,
- oxidative carbonylation
Long Abstrsct
Innovation Points

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References(42)

References

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