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Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming

查看全文 作  者:Wenming [1]Liu;Le [1]Li;Sixue [1]Lin;Yiwei [1]Luo;Zhenghong [2]Bao;Yiru [1]Mao;Kongzhai [3]Li;Daishe [1]Wu;Honggen [1]Peng 高影响力作者 机构地区:[1]College of Chemistry,Key Laboratory of Poyang Lake Environment and Resource Utilization,Ministry of Education,School of Resources Environmental and Chemical Engineering,Nanchang University,Nanchang 330031,Jiangxi,China;[2]Chemical Sciences Divison,Oak Ridge National Laboratory,Oak Ridge,TN 37830,USA;[3]State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering,Kunming University of Science and Technology,Kunming 650093,Yunnan,China高影响力机构 出  处:《Journal of Energy Chemistry》索引2022年第31卷第2期,共14页高影响力期刊 基  金:supported by the National Natural Science Foundation of China(21976078 and 21773106);the National Key R&D Program of China(2016YFC0205900);the Natural Science Foundation of Jiangxi Province(20202ACB213001);National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2019A12)。 摘  要:Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or hydrogen.The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts.Herein,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(In_(x)Ni@SiO_(2))have been prepared and displayed superior coking resistance for DRM reaction.The sample containing 0.5 wt.%of In loading(In_(0.5)Ni@SiO_(2))shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test.The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In.Both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane.The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases. 关 键 词:Methane dry reforming InNi intermetallic alloy Confinement Coking resistance Utilization of greenhouse gases
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