深入探讨金属与载体之间的适度相互作用,以及在热催化甲烷分解过程中通过锰的整合提高 Ni/SiO2 基催化剂的效率

IF 9.9 1区 工程技术 Q1 ENERGY & FUELS Energy Conversion and Management Pub Date : 2024-11-09 DOI:10.1016/j.enconman.2024.119229
Mina Karaminejad , Reza Golhosseini , Fereshteh Meshkani , Patrick Da Costa
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引用次数: 0

摘要

开发一种环境友好型高效催化剂对于生成无 COx 和结构碳的清洁氢气至关重要。甲烷的催化分解技术有助于将天然气转化为这些有价值的产品。为此,通过保持活性位点和调节金属-支撑相互作用(MSI)来开发二氧化硅支撑镍催化剂,激活 CH4 的表面缺陷引起了人们的极大兴趣。因此,本文表明,锰的存在提高了表层 NiO 的还原性,并在镍和支撑物之间产生了适度的相互作用,降低了镍原子周围的电子密度,并通过引入晶格缺陷提高了表面氧物种的存在,从而促进了还原,促进了甲烷在镍表面的解离,提高了反应的活性。根据 TEM 分析,表面形貌显示金属镍分散良好,镍晶体生长受到限制。金属与支撑物之间的强相互作用产生了较高的碳扩散驱动力,为碳纳米纤维(CNF)的生长提供了更多的位点。在保持溶解碳的渗入和 CNFs 的膨胀之间的平衡的同时,通过将碳沉积物引向活性位点的边缘,防止活性位点被覆盖而导致催化剂失活,以及活性氧产生的焦炭氧化,这些都表明锰在催化剂构型中的有效存在。
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Insight into the moderate interaction between the metal and support and reinforcing of Ni/SiO2-based catalysts efficiency with the manganese integration in thermal catalytic methane decomposition
Developing an environmentally friendly and highly efficient catalyst is crucial for generating clean hydrogen without COx and structured carbon. The catalytic decomposition of methane encourages technology to convert natural gas into these valuable products. For this purpose, surface defects in activating CH4 have garnered much interest in developing silica-supported nickel catalysts by maintaining active sites and modulating metal-support interaction (MSI). Thus, It is shown here that the presence of Mn improved the reducibility of superficial NiO and created a moderate interaction between Ni and the support, decreasing the electron density around the Ni atom and elevating surface oxygen species’ presence by introducing lattice defects, thus facilitating the reduction, promoting the dissociation of methane on the nickel surface and enhancing the reactivity of the reaction Consequently, this MSI modulate stabilized the active sites, preventing quick sintering under reaction conditions. Based on TEM analysis, the surface morphology revealed well-dispersed metallic Ni and the restriction of Ni crystal growth. The strong metal-support interaction resulted in a high carbon diffusion driving force, providing more sites for growth in carbon nanofiber (CNFs). Maintaining the balance between the infiltration of dissolved carbon and the expansion of CNFs while also preventing the deactivation of the catalyst due to the covering of active sites by channeling carbon deposits towards the edges of the active sites and oxidation of coke produced by active oxygen species, all showed the effective presence of manganese in the catalyst’s configuration.
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来源期刊
Energy Conversion and Management
Energy Conversion and Management 工程技术-力学
CiteScore
19.00
自引率
11.50%
发文量
1304
审稿时长
17 days
期刊介绍: The journal Energy Conversion and Management provides a forum for publishing original contributions and comprehensive technical review articles of interdisciplinary and original research on all important energy topics. The topics considered include energy generation, utilization, conversion, storage, transmission, conservation, management and sustainability. These topics typically involve various types of energy such as mechanical, thermal, nuclear, chemical, electromagnetic, magnetic and electric. These energy types cover all known energy resources, including renewable resources (e.g., solar, bio, hydro, wind, geothermal and ocean energy), fossil fuels and nuclear resources.
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