High purity H2 resource from methanol steam reforming at low-temperature by spinel CuGa2O4 catalyst for fuel cell

IF 5.1 2区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Ceramics International Pub Date : 2024-09-25 DOI:10.1016/j.ceramint.2024.09.319
Gaokui Chen, Qiuwan Shen, Xin Zhang, Tianyun Zhao, Kuanyu Zhu, Shian Li
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Abstract

Methanol steam reforming (MSR) is an effective way to provide high purity hydrogen for PEMFCs, however the main challenge is the toxic effect of CO. In this study, CuGa2O4 spinel catalyst was applied first for MSR at low temperature. The properties of catalysts were characterized by various techniques, the MSR catalytic performance was also studied in deeply. The surface of the catalyst is composed of particle chains that are interconnected, forming high-volume pores that increase the specific surface area. The catalyst also has a rich porous structure, exposing more active sites. Furthermore, the presence of oxygen vacancies facilitates the adsorption of reactive oxygen species, reducing CO generation. A possible pathway for methanol dehydrogenation has been determined using DFT calculations. The relatively low overall energy barrier on the catalyst surface facilitates methanol activation. Among the steps, formaldehyde dehydrogenation is the rate-determining step in the methanol dehydrogenation process. The CuGa2O4 catalyst exhibits good gas selectivity, with a hydrogen selectivity of 98 % and CO selectivity of 0. and no deactivation occurred within 50 h, demonstrating outstanding durability. These features allow it to serve as an efficient catalyst for MSR online hydrogen production and direct supply to PEMFCs.
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燃料电池用尖晶石 CuGa2O4 催化剂低温蒸汽转化甲醇产生的高纯度 H2 资源
甲醇蒸汽转化(MSR)是为 PEMFC 提供高纯度氢气的有效方法,但主要挑战在于 CO 的毒性效应。本研究首先将 CuGa2O4 尖晶石催化剂用于低温 MSR。通过各种技术对催化剂的特性进行了表征,并对 MSR 催化性能进行了深入研究。催化剂表面由颗粒链组成,颗粒链之间相互连接,形成大体积孔隙,增加了比表面积。催化剂还具有丰富的多孔结构,暴露出更多的活性位点。此外,氧空位的存在有利于吸附活性氧,从而减少 CO 的生成。利用 DFT 计算确定了甲醇脱氢的可能途径。催化剂表面相对较低的总能障有利于甲醇的活化。其中,甲醛脱氢是甲醇脱氢过程中决定速率的步骤。CuGa2O4 催化剂具有良好的气体选择性,氢气选择性为 98%,一氧化碳选择性为 0.0%,且在 50 小时内未发生失活现象,表现出卓越的耐久性。这些特点使其成为 MSR 在线制氢和直接供应 PEMFC 的高效催化剂。
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来源期刊
Ceramics International
Ceramics International 工程技术-材料科学:硅酸盐
CiteScore
9.40
自引率
15.40%
发文量
4558
审稿时长
25 days
期刊介绍: Ceramics International covers the science of advanced ceramic materials. The journal encourages contributions that demonstrate how an understanding of the basic chemical and physical phenomena may direct materials design and stimulate ideas for new or improved processing techniques, in order to obtain materials with desired structural features and properties. Ceramics International covers oxide and non-oxide ceramics, functional glasses, glass ceramics, amorphous inorganic non-metallic materials (and their combinations with metal and organic materials), in the form of particulates, dense or porous bodies, thin/thick films and laminated, graded and composite structures. Process related topics such as ceramic-ceramic joints or joining ceramics with dissimilar materials, as well as surface finishing and conditioning are also covered. Besides traditional processing techniques, manufacturing routes of interest include innovative procedures benefiting from externally applied stresses, electromagnetic fields and energetic beams, as well as top-down and self-assembly nanotechnology approaches. In addition, the journal welcomes submissions on bio-inspired and bio-enabled materials designs, experimentally validated multi scale modelling and simulation for materials design, and the use of the most advanced chemical and physical characterization techniques of structure, properties and behaviour. Technologically relevant low-dimensional systems are a particular focus of Ceramics International. These include 0, 1 and 2-D nanomaterials (also covering CNTs, graphene and related materials, and diamond-like carbons), their nanocomposites, as well as nano-hybrids and hierarchical multifunctional nanostructures that might integrate molecular, biological and electronic components.
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