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H_(2)在Mo_(x)S_(y)团簇上吸附解离的尺寸效应研究 被引量:1
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作者 杜峰 尹思琦 +4 位作者 罗辉 邓文安 李传 黄振薇 王文静 《化工学报》 EI CSCD 北大核心 2022年第9期3895-3903,共9页
浆态床加氢工艺可以处理不同来源的劣质重油、渣油,氢气的活化是重油加氢处理过程中发生的主要反应之一。钼基催化剂的分散性是影响重油加氢活性的关键因素。构建了Mo_(7)S_(15)、Mo_(12)S_(26)、Mo_(18)S_(39)、Mo_(25)S_(54)和Mo_(33)... 浆态床加氢工艺可以处理不同来源的劣质重油、渣油,氢气的活化是重油加氢处理过程中发生的主要反应之一。钼基催化剂的分散性是影响重油加氢活性的关键因素。构建了Mo_(7)S_(15)、Mo_(12)S_(26)、Mo_(18)S_(39)、Mo_(25)S_(54)和Mo_(33)S_(71)团簇,利用密度泛函理论研究了团簇自身的稳定性、活性以及H_(2)在不同尺寸团簇上的吸附与解离过程。结果发现,在目前所建立的团簇中,其尺寸越小,结合能越低,最高占据分子轨道-最低未占分子轨道(HOMOLUMO)能隙值越小,团簇稳定性越弱,活性越强。H_(2)在簇上的稳定吸附位点为边缘位点。随团簇尺寸增大,吸附能分别为-64.25、-34.60、-34.14、-7.20、-6.82 kJ/mol,吸附能绝对值减小,氢气分子与团簇的相互作用减弱,并且解离能逐渐增大,分别为13.76、33.14、53.64、60.75、64.47 kJ/mol。目前的结果表明,团簇尺寸越小,氢气的吸附解离越容易,显示出更高的活性。 展开更多
关键词 mo_(x)s_(y)团簇 团簇尺寸 氢气活化 钼基催化剂 密度泛函理论
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MoS_(x) nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters for efficient electrocatalytic hydrogen evolution
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作者 Haoxuan Yu Junan Pan +7 位作者 Kang Chen Wang Chao Zechao Zhuang Sizhuo Feng Jianmei Chen Lingbin Xie Longlu Wang Qiang Zhao 《Nano Research》 SCIE EI CSCD 2024年第8期6910-6915,共6页
Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))an... Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))and unraveling its structure−activity relationship.By leveraging transition molybdenum polysulfide clusters as functional units for multi-level ordering,we successfully designed and synthesized MoS_(x)nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters via evaporationinduced self-assembly,which exhibit enhanced HER activity attributed to a high density of active sites and dynamic evolution behavior under cathodic potentials.MoS_(x) nanowire networks electrode yields a current density of 100 mA·cm^(−2) at 142 mV in 0.5 M H_(2)SO_(4).This work provides an attractive prospect for optimizing catalysts at the sub-nano scale and offers insights into a strategy for designing catalysts in various gas evolution reactions. 展开更多
关键词 mos_(x) nanowire networks [mo_(3)s_(13)]^(2−)clusters hydrogen evolution reaction(HER) sub-nano scale
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