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Mechanistic study of Cu-Ni bimetallic catalysts supported by graphene derivatives for hydrogenation of CO2 to methanol
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-04-21 , DOI: 10.1016/j.jcou.2021.101542
Chengrui Wang , Yanhong Fang , Guangfen Liang , Xiangyong Lv , Huamei Duan , Yandong Li , Dengfu Chen , Mujun Long

The Cu-Ni bimetallic catalyst supported by graphene derivatives was employed to explore the reaction mechanisms of converting CO2 to methanol. Their properties were analyzed by Raman, XRD, XPS, TG-DSC, TEM and CO2-TPD. Cu or Ni catalyst supported by graphene oxide (GO) tended to combine with defects, leading to less defects of Cu-GO and Ni-GO. So does reduced graphene oxide (rGO). However, ammonia modified graphene (NGO) presented more defects compared to GO and rGO. These changes showed that the functional group and metal ion had been introduced. In addition, more active component (Cu°) could be detected in rGO supported catalyst. In GO and rGO, the addition of Ni could promote the reduction of Cu2+, while Ni showed inhibitory performance in NGO. CuNi-rGO and CuNi-NGO could chemically activate more CO2 at lower temprerature. These catalysts could lower the activation energy of CO2 by 40 %. Most of Ni and Cu dispersed uniformly on supports. In rGO, the size of Cu-Ni was less than 20 nm. In NGO, the size was 50–100 nm. Which means more activation component could been exposed to reactant gas on rGO and it was a better support. Compared with literature, the adsorption capacity of CO2 could increase 76.92 % maximally. In the catalytic test, CuNi-rGO showed a CO2 conversion of 7.87 % and the methanol selectivity of 98.7 % at 498 K and 4.0 MPa, which exhibited a competitive performance compared with other catalysts in literatures.



中文翻译:

石墨烯衍生物负载Cu-Ni双金属催化剂将CO 2加氢制甲醇的机理研究

利用石墨烯衍生物负载的Cu-Ni双金属催化剂探索了CO 2转化为甲醇的反应机理。通过拉曼,XRD,XPS,TG-DSC,TEM和CO 2 -TPD分析了它们的性质。由氧化石墨烯(GO)负载的Cu或Ni催化剂倾向于与缺陷结合,从而导致较少的Cu-GO和Ni-GO缺陷。还原氧化石墨烯(rGO)也是如此。但是,与GO和rGO相比,氨改性石墨烯(NGO)表现出更多的缺陷。这些变化表明已经引入了官能团和金属离子。另外,在rGO负载的催化剂中可以检测到更多的活性成分(Cu°)。在GO和rGO中,添加Ni可以促进Cu 2+的还原,而镍在非政府组织中表现出抑制作用。CuNi-rGO和CuNi-NGO可以在较低的温度下化学活化更多的CO 2。这些催化剂可使CO 2的活化能降低40%。Ni和Cu的大部分均匀地分散在载体上。在rGO中,Cu-Ni的尺寸小于20 nm。在NGO中,大小为50-100 nm。这意味着更多的活化成分可能会在rGO上暴露于反应气体中,这是一个更好的支持。与文献相比,CO 2的吸附量最大增加了76.92%。在催化试验中,CuNi-rGO在498 K和4.0 MPa下的CO 2转化率为7.87%,甲醇选择性为98.7%,与文献中的其他催​​化剂相比,具有竞争优势。

更新日期:2021-04-22
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