首页|期刊导航|燃料化学学报|Ni调控Zn基氧化物催化剂的异丁烷氧化脱氢性能

Ni调控Zn基氧化物催化剂的异丁烷氧化脱氢性能OA北大核心

Modification of Zn-based oxides with Ni substitution and their catalytic performance in the oxidative dehydrogenation of isobutane

中文摘要英文摘要

本工作以ZnNiAl水滑石(ZnNiAl-LDH)为前驱体,通过焙烧和还原处理制备一系列Zn-Ni-Al金属氧化物负载的Zn-Ni双金属催化剂,其中(Zn+Ni)/Al物质的量比为2;系统探究了 Ni取代量(Ni/(Zn+Ni)物质的量比 x=0,0.1,0.5,1.0,2.0)对催化剂结构、织构、表面化学状态、还原能力、酸碱性和CO脱附性能的影响,并关联其对CO2氧化异丁烷(i-C4H10)脱氢(CO2-ODHB)的催化性能.结果表明,Ni的取代可调控相组成和还原能力,优化孔道结构并稳定其对CO2-ODHB的催化性能等.微量Ni取代(x=0.1)有助于构建Zn-Ni-Al的相互作用,获得适宜的表面酸性和弱碱性,抑制积炭并促进CO脱附及积炭的消除,使i-C4H10转化率稳定在41%以上,i-C4H8选择性达90%.然而过量Ni取代(x≥0.5)则会导致Zn-Ni-Al催化剂的酸性过强和CO2竞争吸附加剧副反应,致使CH4选择性显著上升.

A series of ZnNiAl metal oxide-supported Zn-Ni bimetallic catalysts were prepared by roasting and reduction treatment using ZnNiAl hydrotalcite(ZnNiAl-LDH)as a precursor,which had a fixed(Zn+Ni)/Al molar ratio of 2 but varied in the Ni/(Zn+Ni)molar ratio(x=0,0.1,0.5,1.0,2.0).The effect of Ni substitution content on the structure,texture,surface chemical state,reducing ability,acidity and alkalinity and CO desorption properties of the Ni-Zn-Al catalysts were systematically explored,in connection with their catalytic performance in the oxidative dehydrogenation of isobutane(i-C4H10)with CO2(CO2-ODHB).The results indicate that Ni can control the composition and reduction ability of the substituted phase,optimize the pore structure and stabilize the catalytic performance in CO2-ODHB.Trace Ni substitution(x=0.1)helps to establish appropriate Zn-Ni-Al interactions in the ZNA-0.1-R catalyst,achieving suitable surface acidity and weak alkalinity,inhibiting carbon deposition and promoting the CO desorption and the elimination of carbon deposition,over which the conversion of i-C4H10 is stable(>41%)with a selectivity of 90%to i-C4H8.However,excessive Ni substitution(x ≥ 0.5)can aggravate the side reaction due to excessive acidity and competitive adsorption of CO2,resulting in a significant increase in the selectivity to CH4.

孙婷婷;张立红;王蕊蕊;贾镕婧;徐梦烁;薛洋洋;肖璨;邵张璋;徐彦红;薛定

天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350天津大学化工学院,天津 300350平顶山学院化学与环境工程学院,河南平顶山 467000天津市工业尾气资源综合利用技术工程中心,天津 300271

化学

CO2异丁烷脱氢催化剂水滑石Ni取代量

CO2isobutanedehydrogenationcatalysthydrotalciteNi substitution

《燃料化学学报》 2025 (11)

1628-1640,13

The project was supported by National Natural Science Foundation of China(21776214).国家自然科学基金(21776214)资助

10.1016/S1872-5813(25)60578-0

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