当前位置: X-MOL 学术J. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
The promoting role of Ga in ZnZrOx solid solution catalyst for CO2 hydrogenation to methanol
Journal of Catalysis ( IF 6.5 ) Pub Date : 2021-10-07 , DOI: 10.1016/j.jcat.2021.09.030
Feng Sha 1, 2 , Chizhou Tang 2, 3 , Shan Tang 2, 3 , Qingnan Wang 2 , Zhe Han 1, 2 , Jijie Wang 2 , Can Li 2
Affiliation  

Catalytic conversion of CO2 into methanol utilizing green hydrogen produced from renewable energy is a promising route to realize carbon neutrality. Although ZnZrOx solid solution catalyst displays excellent catalytic performance, it is still highly desired to make any further improvement. Herein, we found the promoting effect of incorporating Ga into ZnZrOx solid solution catalyst in CO2 hydrogenation to methanol. Ga promoted ZnZrOx (GaZnZrOx) solid solution catalyst exhibits CO2 conversion of 8.8% and methanol space time yield of 630 mg gcat−1 h−1 that are higher than those of ZnZrOx solid solution catalyst (7.7%, 556 mg gcat−1 h−1) at 320 °C, while the highly selectivity toward methanol remains unchanged. Chemisorption and H2-D2 exchange results show that GaZnZrOx solid solution catalyst displays higher capacity for the adsorption and activation of H2 than ZnZrOx solid solution catalyst. Electron paramagnetic resonance result suggests that more oxygen vacancies are derived after incorporating Ga into ZnZrOx solid solution catalyst. In situ diffuse reflectance infrared Fourier transform spectra indicate that the HCOO* and CH3O* species are the main intermediate species. The higher IR intensity of intermediate species and lower CH3O*/HCOO* ratio on GaZnZrOx solid solution catalyst suggest that the hydrogenation of HCOO* to CH3O* is boosted. These results reveal the promoting effect of incorporated Ga into ZnZrOx solid solution catalyst that improves the adsorption and activation of H2 and CO2, thus enhancing catalytic performance of methanol synthesis from CO2 hydrogenation.



中文翻译:

Ga在ZnZrOx固溶体催化剂CO2加氢制甲醇中的促进作用

利用可再生能源产生的绿色氢将 CO 2催化转化为甲醇是实现碳中和的有前景的途径。尽管ZnZrO x固溶体催化剂表现出优异的催化性能,但仍需进一步改进。在此,我们发现了将Ga掺入ZnZrO x固溶体催化剂中对CO 2加氢制甲醇的促进作用。Ga促进的ZnZrO x (GaZnZrO x )固溶体催化剂的CO 2转化率为8.8%,甲醇时空产率为630 mg g cat -1  h -1,高于ZnZrOx固溶体催化剂 (7.7%, 556 mg g cat -1  h -1 ) 在 320 °C,而对甲醇的高度选择性保持不变。化学吸附和H 2 -D 2交换结果表明,GaZnZrO X固溶体催化剂显示更高的容量为H的吸附和活化2比ZnZrO X固溶体催化剂。电子顺磁共振结果表明在将Ga掺入ZnZrO x固溶体催化剂后产生更多的氧空位。原位漫反射红外傅立叶变换光谱表明 HCOO* 和 CH 3O* 物种是主要的中间物种。GaZnZrO x固溶体催化剂上中间物种的较高IR强度和较低的CH 3 O*/HCOO*比表明HCOO*加氢为CH 3 O*的过程得到促进。这些结果揭示了将Ga掺入ZnZrO x固溶体催化剂中的促进作用,提高了H 2和CO 2的吸附和活化,从而提高了CO 2加氢合成甲醇的催化性能。

更新日期:2021-11-02
down
wechat
bug