Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

doi:10.1016/j.cjche.2023.07.014

中国化学工程学报 ›› 2024, Vol. 68 ›› Issue (4): 241-252.DOI: 10.1016/j.cjche.2023.07.014

Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

Yunyu Guo¹, Yiran Wang¹, Shu Zhang², Yi Wang³, Song Hu³, Jun Xiang³, Walid Nabgan⁴, Xun Hu¹

1. School of Material Science and Engineering, University of Jinan, Jinan 250022, China;
2. Joint International Research Laboratory of Biomass Energy and Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China;
3. State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China;
4. Departament d'Enginyeria Química, Universitat Rovira i Virgili, Tarragona 43007, Spain

收稿日期:2023-03-26 修回日期:2023-07-07 出版日期:2024-04-28 发布日期:2024-06-28
通讯作者: Xun Hu,Tel./Fax:+86 531 89736201.E-mail address:Xun.Hu@outlook.com
基金资助:
This work was supported by National Natural Science Foundation of China (51876080), the Program for Taishan Scholars of Shandong Province Government, the Agricultural Innovation Program of Shandong Province (SD2019NJ015) and the Research and Development program of Shandong Basan Graphite New Material Plant, National Natural Science Foundation of China (52076097), Key projects for inter-governmental cooperation in international science, technology and innovation (2018YFE0127500).

Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

Yunyu Guo¹, Yiran Wang¹, Shu Zhang², Yi Wang³, Song Hu³, Jun Xiang³, Walid Nabgan⁴, Xun Hu¹

1. School of Material Science and Engineering, University of Jinan, Jinan 250022, China;
2. Joint International Research Laboratory of Biomass Energy and Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China;
3. State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China;
4. Departament d'Enginyeria Química, Universitat Rovira i Virgili, Tarragona 43007, Spain

Received:2023-03-26 Revised:2023-07-07 Online:2024-04-28 Published:2024-06-28
Contact: Xun Hu,Tel./Fax:+86 531 89736201.E-mail address:Xun.Hu@outlook.com
Supported by:
This work was supported by National Natural Science Foundation of China (51876080), the Program for Taishan Scholars of Shandong Province Government, the Agricultural Innovation Program of Shandong Province (SD2019NJ015) and the Research and Development program of Shandong Basan Graphite New Material Plant, National Natural Science Foundation of China (52076097), Key projects for inter-governmental cooperation in international science, technology and innovation (2018YFE0127500).

摘要/Abstract

摘要： Biochar is a reactive carrier as it may be partially gasified with steam in steam reforming, which could influence the formation of reaction intermediates and modify catalytic behaviors. Herein, the Ni/biochar as well as two comparative catalysts, Ni/Al₂O₃ and Ni/SiO₂, with low nickel loading (2% (mass)) was conducted to probe involvement of the varied carriers in the steam reforming. The results indicated that the Ni/biochar performed excellent catalytic activity than Ni/SiO₂ and Ni/Al₂O₃, as the biochar carrier facilitated quick conversion of the -OH from dissociation of steam to gasify the oxygen-rich carbonaceous intermediates like C=O and C-O-C, resulting in low coverage while high exposure of nickel species for maintaining the superior catalytic performance. In converse, strong adsorption of aliphatic intermediates over Ni/Al₂O₃ and Ni/SiO₂ induced serious coking with polymeric coke as the main type (21.5% and 32.1%, respectively), which was significantly higher than that over Ni/biochar (3.9%). The coke over Ni/biochar was mainly aromatic or catalytic type with nanotube morphology and high crystallinity. The high resistivity of Ni/biochar towards coking was due to the balance between formation of coke and gasification of coke and partially biochar with steam, which created developed mesopores in spent Ni/biochar while the coke blocked pores in Ni/Al₂O₃ and Ni/SiO₂ catalysts.

关键词: Steam reforming, Acetic acid, Ni/biochar catalyst, Property of coke, Reaction intermediates

Abstract: Biochar is a reactive carrier as it may be partially gasified with steam in steam reforming, which could influence the formation of reaction intermediates and modify catalytic behaviors. Herein, the Ni/biochar as well as two comparative catalysts, Ni/Al₂O₃ and Ni/SiO₂, with low nickel loading (2% (mass)) was conducted to probe involvement of the varied carriers in the steam reforming. The results indicated that the Ni/biochar performed excellent catalytic activity than Ni/SiO₂ and Ni/Al₂O₃, as the biochar carrier facilitated quick conversion of the -OH from dissociation of steam to gasify the oxygen-rich carbonaceous intermediates like C=O and C-O-C, resulting in low coverage while high exposure of nickel species for maintaining the superior catalytic performance. In converse, strong adsorption of aliphatic intermediates over Ni/Al₂O₃ and Ni/SiO₂ induced serious coking with polymeric coke as the main type (21.5% and 32.1%, respectively), which was significantly higher than that over Ni/biochar (3.9%). The coke over Ni/biochar was mainly aromatic or catalytic type with nanotube morphology and high crystallinity. The high resistivity of Ni/biochar towards coking was due to the balance between formation of coke and gasification of coke and partially biochar with steam, which created developed mesopores in spent Ni/biochar while the coke blocked pores in Ni/Al₂O₃ and Ni/SiO₂ catalysts.

Key words: Steam reforming, Acetic acid, Ni/biochar catalyst, Property of coke, Reaction intermediates

Yunyu Guo, Yiran Wang, Shu Zhang, Yi Wang, Song Hu, Jun Xiang, Walid Nabgan, Xun Hu. Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance[J]. 中国化学工程学报, 2024, 68(4): 241-252.

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Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

Steam reforming of acetic acid over Ni/biochar of low metal-loading: Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

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