Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation

doi:10.1016/j.cjche.2021.11.004

Chinese Journal of Chemical Engineering ›› 2022, Vol. 48 ›› Issue (8): 176-190.DOI: 10.1016/j.cjche.2021.11.004

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Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation

Yishuang Wang¹, Na Li¹, Mingqiang Chen¹, Defang Liang¹, Chang Li², Quan Liu², Zhonglian Yang¹, Jun Wang¹

1. School of Chemical Engineering, Anhui University of Science and Technology, Huainan 232001, China;
2. Analytical and Testing Center, Anhui University of Science and Technology, Huainan 232001, China

Received:2021-07-06 Revised:2021-11-01 Online:2022-09-30 Published:2022-08-28
Contact: Mingqiang Chen,E-mail:mqchen@aust.edu.cn
Supported by:
The authors would be grateful for the financial assistance from the National Natural Science Foundation of China (51906001 and 51876001), University Natural Science Research Project of Anhui Province (KJ2020ZD31), Key Research and Development Projects of Anhui Province (202004a06020053) and Doctoral Fund project of Anhui University of Science and Technology. We would also be grateful for the technological support of characterizations from the Analysis and Testing Center of Anhui University of Science and Technology.

Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation

Yishuang Wang¹, Na Li¹, Mingqiang Chen¹, Defang Liang¹, Chang Li², Quan Liu², Zhonglian Yang¹, Jun Wang¹

1. School of Chemical Engineering, Anhui University of Science and Technology, Huainan 232001, China;
2. Analytical and Testing Center, Anhui University of Science and Technology, Huainan 232001, China

通讯作者: Mingqiang Chen,E-mail:mqchen@aust.edu.cn
基金资助:
The authors would be grateful for the financial assistance from the National Natural Science Foundation of China (51906001 and 51876001), University Natural Science Research Project of Anhui Province (KJ2020ZD31), Key Research and Development Projects of Anhui Province (202004a06020053) and Doctoral Fund project of Anhui University of Science and Technology. We would also be grateful for the technological support of characterizations from the Analysis and Testing Center of Anhui University of Science and Technology.

Abstract

Abstract: Glycerol steam reforming (GSR) is one of the promising technologies that can realize renewable hydrogen production and efficient utilization of crude glycerol. To illuminate the functions of Ca content (3%, 6%, 9%, and 12%, by mass) and preparation method for Ni/ATP catalyst structure and its catalytic behaviors, the Ni-xCa/ATP (x?=?3%, 6%, 9%, and 12%, by mass) catalysts are prepared by co-impregnation (ci) and hydrothermal synthesis (hs) method and then tested in GSR. Characterization results of XRD, N₂ adsorption–desorption, H₂-TPR, HRTEM, XPS, and NH₃/CO₂-TPD demonstrate that the combined effect between appropriate Ca additive (6%, by mass) and hs enhance catalyst reducibility, uniform distribution of Ca additive and nickel species over ATP, and adsorption for CO₂. This attributes to hs method protects the ATP framework through suppressing the interaction of Ca with ATP and promotes the formation of Ni-CaO interface sites. Therefore, Ni-6Ca/ATP-hs exhibits the highest conversion (86.77%) of glycerol to gas product and H₂ yield (76.17%) and selectivity (58.56%) during GSR. Furthermore, XRD, HRTEM, TG-DTG and Raman analyses confirm that Ni-6Ca/ATP-hs also reveals outstanding anti-sintering and coke resistance. In addition, the structural evolution process of Ni/ATP catalyst with Ca introduction and hs method is presented. Considering the high performance, simple preparation process and low cost, the as-prepared catalyst providing new opportunities for utilization of glycerol derived from biodiesel industry.

Key words: Hydrogen production, Catalysis, Renewable energy, Steam reforming of glycerol, Attapulgite, Nickel catalyst

摘要： Glycerol steam reforming (GSR) is one of the promising technologies that can realize renewable hydrogen production and efficient utilization of crude glycerol. To illuminate the functions of Ca content (3%, 6%, 9%, and 12%, by mass) and preparation method for Ni/ATP catalyst structure and its catalytic behaviors, the Ni-xCa/ATP (x?=?3%, 6%, 9%, and 12%, by mass) catalysts are prepared by co-impregnation (ci) and hydrothermal synthesis (hs) method and then tested in GSR. Characterization results of XRD, N₂ adsorption–desorption, H₂-TPR, HRTEM, XPS, and NH₃/CO₂-TPD demonstrate that the combined effect between appropriate Ca additive (6%, by mass) and hs enhance catalyst reducibility, uniform distribution of Ca additive and nickel species over ATP, and adsorption for CO₂. This attributes to hs method protects the ATP framework through suppressing the interaction of Ca with ATP and promotes the formation of Ni-CaO interface sites. Therefore, Ni-6Ca/ATP-hs exhibits the highest conversion (86.77%) of glycerol to gas product and H₂ yield (76.17%) and selectivity (58.56%) during GSR. Furthermore, XRD, HRTEM, TG-DTG and Raman analyses confirm that Ni-6Ca/ATP-hs also reveals outstanding anti-sintering and coke resistance. In addition, the structural evolution process of Ni/ATP catalyst with Ca introduction and hs method is presented. Considering the high performance, simple preparation process and low cost, the as-prepared catalyst providing new opportunities for utilization of glycerol derived from biodiesel industry.

关键词: Hydrogen production, Catalysis, Renewable energy, Steam reforming of glycerol, Attapulgite, Nickel catalyst

Yishuang Wang, Na Li, Mingqiang Chen, Defang Liang, Chang Li, Quan Liu, Zhonglian Yang, Jun Wang. Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation[J]. Chinese Journal of Chemical Engineering, 2022, 48(8): 176-190.

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Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation

Glycerol steam reforming over hydrothermal synthetic Ni-Ca/attapulgite for green hydrogen generation

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