首页|固载Cu(Ⅰ)的π络合MOF吸附剂用于乙烷/乙烯的选择性分离

固载Cu(Ⅰ)的π络合MOF吸附剂用于乙烷/乙烯的选择性分离

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金属有机框架材料作为常见的吸附剂,已被广泛地应用于乙烷和乙烯气体混合物的分离,其中引入金属离子所产生π-络合作用可以显著提高MOFs对乙烯的吸附能力.在双羟基功能化后的UiO-66中负载Cu(Ⅰ),得到了优先吸附乙烯的Cu(Ⅰ)@UiO-66-(OH)2吸附剂.羟基功能化的框架在增强极性的同时,可以与Cu(Ⅰ)产生协同效应,有效地提高了材料对乙烯/乙烷的吸附分离性能.得到的3%(质量分数)Cu(Ⅰ)@UiO-66-(OH)2在298 K及1 bar(1 bar=0.1 MPa)条件下的C2H4/C2H6IAST选择性为2.98,约为纯UiO-66-(OH)2 的 3倍.单组分吸附实验证明3%Cu(Ⅰ)@UiO-66-(OH)2在整个压力范围下对乙烯的吸附容量均高于乙烷,并且其对乙烯的吸附热(42.81 kJ·mol-1)低于许多已报道的乙烯-选择性吸附剂.在模拟工业条件下对50/50(体积比)C2H4/C2H6混合物进行穿透实验,进一步表明了 3%Cu(Ⅰ)@UiO-66-(OH)2吸附剂可以有效分离乙烷/乙烯混合物.
Immobilize Cu(Ⅰ)into π-complexed MOF adsorbent for selectivity separation of ethane/ethylene
As a common adsorbent,metal-organic frameworks(MOFs)has been widely researched in the separation of ethane and ethylene gas mixtures,and the π-complexation generated by the introduction of metal ions can significantly improve the adsorption capacity of MOFs for ethylene.Cu(Ⅰ)was loaded into the dihydroxyl-functionalized UiO-66,and a Cu(Ⅰ)@UiO-66-(OH)2 adsorbent that preferentially adsorbed ethylene was obtained.The hydroxyl functionalized framework has a synergistic effect with Cu(Ⅰ)while enhancing the polarity,which can effectively improve the adsorption and separation performance of ethylene/ethane.The calculated C2H4/C2H6 IAST selectivity of 3%(mass)Cu(Ⅰ)@UiO-66-(OH)2 at 298 K and 1 bar is 2.98,which is approximately 3 times of the original UiO-66-(OH)2.Single-component adsorption experiments show that the adsorption capacity of 3%Cu(Ⅰ)@UiO-66-(OH)2 for ethylene is higher than that of ethane in the whole pressure range,and its adsorption heat of ethylene(42.81 kJ·mol-1)is lower than that of many reported ethylene-selective adsorbents.The breakthrough experiments of 50/50(volume ratio)C2H4/C2H6 mixture under simulated industrial conditions further demonstrate that the 3%Cu(Ⅰ)@UiO-66-(OH)2 adsorbent can effectively separate the ethane/ethylene mixture.

ethaneethyleneadsorptionadsorbentselectivityπ-complexation

王涛虹、王超、李政、刘莹、田歌、常刚刚、阳晓宇、鲍宗必

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武汉理工大学化学化工与生命科学学院,湖北武汉 430070

浙江大学化学工程与生物工程学院,浙江杭州 310027

乙烷 乙烯 吸附 吸附剂 选择性 π-络合作用

国家重点研发计划项目湖北省重点研发计划项目湖北省青年拔尖人才培养计划项目

2022YFB38068002023BAB101

2024

化工学报
中国化工学会 化学工业出版社

化工学报

CSTPCD北大核心
影响因子:1.26
ISSN:0438-1157
年,卷(期):2024.75(7)