Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol

Shunzheng Zhao; Yanfeng Wen; Xianyun Peng; Yuying Mi; Xijun Liu; Yifan Liu; Longchao Zhuo; Guangzhi Hu; Jun Luo; Xiaolong Tang

doi:10.1039/d0ta00190b

Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol

Shunzheng Zhao, Yanfeng Wen, Xianyun Peng, Yuying Mi, Xijun Liu, Yifan Liu, Longchao Zhuo, Guangzhi Hu, Jun Luo, Xiaolong Tang

Research output: Contribution to journal › Article › peer-review

34 Scopus citations

Abstract

The direct electrochemical conversion of noxious formaldehyde into value-added chemicals is a quite promising technique for resolving the increasingly serious environmental issue arising from industrial formaldehyde-containing wastewater. However, thus far, it has not been examined, to the best of our knowledge. This study reports the electrocatalytic hydrogenation of formaldehyde to methanol in a neutral aqueous medium under ambient conditions over a Pt single-atom catalyst, and this catalyst exhibits a favorable methanol yield rate and a high faradaic efficiency of 30.7 mg h^-1 mg_cat.^-1 and 95.8% at -0.8 V versus the reversible hydrogen electrode in 0.1 M Na₂SO₄. Also, it exhibits excellent durability. Atomic-scale structural characterization and theoretical calculations revealed that the above-mentioned efficient performance is related to atomically dispersed Pt-O sites, which could lower the free-energy change for the chemisorption of formaldehyde and activate the C-H bond.

Original language	English
Pages (from-to)	8913-8919
Number of pages	7
Journal	Journal of Materials Chemistry A
Volume	8
Issue number	18
DOIs	https://doi.org/10.1039/d0ta00190b
State	Published - May 14 2020
Externally published	Yes

Funding

This work was nancially supported by the National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (21601136, 51808037, 51971157, and 51761165012), Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), and Science & Technology Development Fund of Tianjin Education Commission for Higher Education (2018KJ126). This work made use of the resources of the Wuxi Research Institute of Applied Technologies of Tsing-hua University. The authors wish to thank facility support at the 1W1B beamline of the Beijing Synchrotron Radiation Facility (BSRF) and Beijing Super Cloud Computing Center.

Funders	Funder number
Science & Technology Development Fund of Tianjin Education Commission for Higher Education	2018KJ126
Tianjin Science Fund for Distinguished Young Scholars	19JCJQJC61800
National Natural Science Foundation of China	21601136, 51761165012, 51808037, 51971157
National Key Research and Development Program of China	2017YFA0700104

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10.1039/d0ta00190b

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title = "Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol",

abstract = "The direct electrochemical conversion of noxious formaldehyde into value-added chemicals is a quite promising technique for resolving the increasingly serious environmental issue arising from industrial formaldehyde-containing wastewater. However, thus far, it has not been examined, to the best of our knowledge. This study reports the electrocatalytic hydrogenation of formaldehyde to methanol in a neutral aqueous medium under ambient conditions over a Pt single-atom catalyst, and this catalyst exhibits a favorable methanol yield rate and a high faradaic efficiency of 30.7 mg h-1 mgcat.-1 and 95.8% at -0.8 V versus the reversible hydrogen electrode in 0.1 M Na2SO4. Also, it exhibits excellent durability. Atomic-scale structural characterization and theoretical calculations revealed that the above-mentioned efficient performance is related to atomically dispersed Pt-O sites, which could lower the free-energy change for the chemisorption of formaldehyde and activate the C-H bond.",

author = "Shunzheng Zhao and Yanfeng Wen and Xianyun Peng and Yuying Mi and Xijun Liu and Yifan Liu and Longchao Zhuo and Guangzhi Hu and Jun Luo and Xiaolong Tang",

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doi = "10.1039/d0ta00190b",

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T1 - Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol

AU - Zhao, Shunzheng

AU - Wen, Yanfeng

AU - Peng, Xianyun

AU - Mi, Yuying

AU - Liu, Xijun

AU - Liu, Yifan

AU - Zhuo, Longchao

AU - Hu, Guangzhi

AU - Luo, Jun

AU - Tang, Xiaolong

PY - 2020/5/14

Y1 - 2020/5/14

N2 - The direct electrochemical conversion of noxious formaldehyde into value-added chemicals is a quite promising technique for resolving the increasingly serious environmental issue arising from industrial formaldehyde-containing wastewater. However, thus far, it has not been examined, to the best of our knowledge. This study reports the electrocatalytic hydrogenation of formaldehyde to methanol in a neutral aqueous medium under ambient conditions over a Pt single-atom catalyst, and this catalyst exhibits a favorable methanol yield rate and a high faradaic efficiency of 30.7 mg h-1 mgcat.-1 and 95.8% at -0.8 V versus the reversible hydrogen electrode in 0.1 M Na2SO4. Also, it exhibits excellent durability. Atomic-scale structural characterization and theoretical calculations revealed that the above-mentioned efficient performance is related to atomically dispersed Pt-O sites, which could lower the free-energy change for the chemisorption of formaldehyde and activate the C-H bond.

AB - The direct electrochemical conversion of noxious formaldehyde into value-added chemicals is a quite promising technique for resolving the increasingly serious environmental issue arising from industrial formaldehyde-containing wastewater. However, thus far, it has not been examined, to the best of our knowledge. This study reports the electrocatalytic hydrogenation of formaldehyde to methanol in a neutral aqueous medium under ambient conditions over a Pt single-atom catalyst, and this catalyst exhibits a favorable methanol yield rate and a high faradaic efficiency of 30.7 mg h-1 mgcat.-1 and 95.8% at -0.8 V versus the reversible hydrogen electrode in 0.1 M Na2SO4. Also, it exhibits excellent durability. Atomic-scale structural characterization and theoretical calculations revealed that the above-mentioned efficient performance is related to atomically dispersed Pt-O sites, which could lower the free-energy change for the chemisorption of formaldehyde and activate the C-H bond.

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JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

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ER -

Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol

Abstract

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