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Ni/Hydrochar Nanostructures Derived from Biomass as Catalysts for H-2 Production through Aqueous-Phase Reforming of Methanol
Gai, Chao; Wang, Xia; Liu, Jinghai; Liu, Zhengang; Ok, Yong Sik; Liu, Wen; Yip, Alex C. K.
2021-09-24
Source PublicationACS APPLIED NANO MATERIALS
ISSN2574-0970
Volume4Issue:9Pages:8958-8971
AbstractAqueous-phase reforming of organic molecules to hydrogen is a promising strategy to address the production and storage of sustainable hydrogen with lower costs; however, the synthesis of inexpensive transition metal (TM) catalysts with desirable activity and stability for the reaction is still challenging. In this work, a green and efficient approach for modulating the geometric/electronic structure of metal/hydrochar nanocomposites from sustainable biomass was proposed for enhancing H-2 production via aqueous-phase reforming of methanol (APRM). A Ni/HC nanocomposite with a special thistle (a perennial species of flowering plant)-like three-dimensional (3D) architecture was first constructed as a model catalyst to expatiate the critical role of modulating an ordered mesoporous structure and interface electron transfer for enhancing APRM. Deliberately balancing heteroatom doping and soft templates contribute to the successful fabrication of the thistle-like superstructure, and such hierarchically porous architectures demonstrated efficient catalysis for APRM, owing to their unique properties, including a highly uniform morphology, narrow partide size distribution, and mesoporous texture with excellent accessibility. In addition, the experimental investigation and density functional theory calculations both substantiated that the combination of heteroatom doping and soft templates was beneficial for the strong electronic metal-support interaction (EMSI) of the metal/hydrochar nanocomposite, which leads to enhanced methanol adsorption, activation, and subsequently improved APRM performance. The electronic structure of the metal/hydrochar nanocomposite played a more significant effect on the intrinsic APRM activity than the geometric structure like the formation of the thistle-like superstructure. Benefiting from the tailored electronic and geometric structure, the resulting Ni-0.1/HC-N-1.5-S-1 catalyst exhibited an unprecedented average turnover frequency (TOF) of 89.5 mol(H2)/mol(Ni)/min, higher than any other known platinum group metal-free catalysts, approaching the reactivity of the state-of-the-art noble metal-based APRM catalysts, while showing excellent stability over 10 consecutive reaction cycles.
Department固体废弃物处理与资源化实验室
Keywordclean and affordable energy biochar pyrolysis hydrogen society hydrothermal carbonization metal-support interaction supported metal catalysts heteroatom doping
WOS Research AreaNanoscience & Nanotechnology ; Materials Science, Multidisciplinary
Document Type期刊论文
Identifierhttps://ir.rcees.ac.cn/handle/311016/45632
Collection固体废弃物处理与资源化实验室
Affiliation1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Inner Mongolia Univ Nationalities, Nano Innovat Inst, Inner Mongolia Key Lab Carbon Nanomat, Tongliao 028000, Peoples R China
4.Nanyang Technol Univ, Sch Chem & Biomed Engn, Singapore 637459, Singapore
5.Univ Canterbury, Dept Chem & Proc Engn, Christchurch 4800, New Zealand
6.Korea Univ, Korea Biochar Res Ctr, APRU Sustainable Waste Management, Seoul 02841, South
Recommended Citation
GB/T 7714
Gai, Chao,Wang, Xia,Liu, Jinghai,et al. Ni/Hydrochar Nanostructures Derived from Biomass as Catalysts for H-2 Production through Aqueous-Phase Reforming of Methanol[J]. ACS APPLIED NANO MATERIALS,2021,4(9):8958-8971.
APA Gai, Chao.,Wang, Xia.,Liu, Jinghai.,Liu, Zhengang.,Ok, Yong Sik.,...&Yip, Alex C. K..(2021).Ni/Hydrochar Nanostructures Derived from Biomass as Catalysts for H-2 Production through Aqueous-Phase Reforming of Methanol.ACS APPLIED NANO MATERIALS,4(9),8958-8971.
MLA Gai, Chao,et al."Ni/Hydrochar Nanostructures Derived from Biomass as Catalysts for H-2 Production through Aqueous-Phase Reforming of Methanol".ACS APPLIED NANO MATERIALS 4.9(2021):8958-8971.
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