Carbon dioxide hydrogenation to methanol over Cu/ZrO2/CNTs: effect of carbon surface chemistry
Carbon dioxide hydrogenation to methanol over Cu/ZrO2/CNTs: effect of carbon surface chemistry
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DOI：
10.1039/c5ra04774a
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发表时间：
2015-05
期刊：
影响因子：
3.9
通讯作者：
Guannan Wang;Limin Chen;Yuhai Sun;Junliang Wu;Mingli Fu;D. Ye
中科院分区：
文献类型：
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作者：
Guannan Wang;Limin Chen;Yuhai Sun;Junliang Wu;Mingli Fu;D. Ye
在固定床平推流反应器中，考察了不同官能团碳纳米管负载Cu-ZrO 2催化剂的CO2加氢合成甲醇性能。甲醇活性最高（转换频率1.61 × 10 - 2 s-1，时空产率84.0 mg gcat-1 h-1）在Cu/ZrO 2/CNT催化剂上获得在260 ℃、3.0MPa、V（H2）：V（CO2）：V（N2）= 69：1的反应条件下，制备了具有由含氮基团官能化的CNT和仅约10.3wt%的Cu负载量的（CZ/CNT-3）。二十三日：8，GHSV为3600 h-1。采用N2物理吸附、X射线光电子能谱（XPS）、X射线衍射（XRD）、H2程序升温还原（H2-TPR）和H2程序升温脱附（H2-TPD）等技术对催化剂进行了表征。CZ/CNT-3的优异性能归因于碳纳米管表面含氮基团的存在，增加了铜氧化物的分散，促进了其还原，减小了铜的晶粒尺寸，增强了H2和CO2的吸附能力，从而导致了良好的甲醇合成催化性能。
Methanol synthesis from CO2 hydrogenation in a fixed-bed plug flow reactor was investigated over Cu–ZrO2 catalysts supported on CNTs bearing various functional groups. The highest methanol activity (turnover frequency 1.61 × 10−2 s−1, space time yield 84.0 mg gcat−1 h−1) was obtained over the Cu/ZrO2/CNTs catalyst (CZ/CNT-3) with CNTs functionalized by nitrogen-containing groups and Cu loading only about 10.3 wt% under the reaction conditions of 260 °C, 3.0 MPa, V(H2) : V(CO2) : V(N2) = 69 : 23 : 8 and GHSV of 3600 h−1. The catalysts were fully characterized by N2 physisorption, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), H2-temperature-programmed reduction (H2-TPR) and temperature-programmed desorption of H2 (H2-TPD) techniques. The excellent performance of CZ/CNT-3 is attributed to the presence of nitrogen-containing groups on the CNTs surface, which increase the dispersion of copper oxides, promote their reduction, decreases the crystal size of Cu, and enhances H2 and CO2 adsorption capability, thus leading to good catalytic performance towards methanol synthesis.