文章摘要
李静静,刘家旭,荣泽明.改性纳米多孔钴低温催化二氧化碳加氢制甲醇[J].精细化工,2020,37(11):
改性纳米多孔钴低温催化二氧化碳加氢制甲醇
Low Temperature CO2 Hydrogenation to CH3OH over Modified Nanoporous Cobalt Catalyst
投稿时间:2020-06-24  修订日期:2020-07-13
DOI:
中文关键词: 二氧化碳  加氢  甲醇  纳米多孔  
英文关键词: CO2  hydrogenation  CH3OH  nanoporous  Co
基金项目:
作者单位E-mail
李静静 大连理工大学 jingjingli0926@163.com 
刘家旭 大连理工大学  
荣泽明 大连理工大学 zeming@dlut.edu.cn 
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中文摘要:
      低温条件下二氧化碳(CO2)加氢制甲醇(CH3OH)被认为是一项重要且仍具挑战性的工作,本文制备了纳米多孔钴(NP-Co)及改性纳米多孔钴NP-CoxM(M=Cr,V,Mo,Mn,Ce,W,x=nCo∶nM)催化剂,评价其在60-140 ℃的温和条件下催化CO2加氢制CH3OH,铬作为改性元素显著提高了催化剂性能。采用N2-物理吸脱附、SEM、TEM、XRD、XPS和CO2-TPD对NP-Co、NP-Co3Cr进行表征,结果显示CrxO作为改性组分显著增强了CO2与活性位点之间的强相互作用、表面羟基的大量增加促进了CO2低温活化,具体表现为采用NP-Co3Cr的表观活化能(59.08 kJ/mol)相比NP-Co(89.12 kJ/mol)显著降低。CH3OH作为主要产物,其60 ℃下的时间收率为106.4 μmol/(gCat.·h)且选择性达92.8%,相同反应条件下的NP-Co则未观察到CH3OH生成。
英文摘要:
      CO2 hydrogenation to CH3OH under relatively lower temperature has considered an important but still challenging task. Herein, nanoporous Co (NP-Co) and a series of modified NP-CoxM (M=Cr, V, Mo, Mn, Ce, W, x=nCo∶nM) were synthesized and evaluated for CO2 hydrogenation to CH3OH at 60-140 °C. Cr element as an additive seems to be favorable for the promotion of catalytic performance. N2 adsorption-desorption, SEM, TEM, XRD, XPS and CO2-TPD were employed for the characterization of NP-Co and NP-CoCrx. Results showed the addition of CrOx enhanced the strong interaction between CO2 and the catalytic active site. In addition, the large increase of surface hydroxyl promoted the activation of CO2 under relatively lower temperature, which was manifested as the significant reduction of apparent activation energy for NP-Co3Cr (59.08 kJ/mol) compared with NP-Co (89.12 kJ/mol). CH3OH as a major product exhibited time yield of 106.4 μmol/(gCat.·h) at 60 °C and selectivity was up to 92.8%, while no CH3OH generated with NP-Co catalyst under the same reaction conditions.
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