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嵌入超低含量氧化锌量子点的碳包覆氧化铟中空管作为一氧化碳加氢制甲醇的催化剂。

Carbon coated InO hollow tubes embedded with ultra-low content ZnO quantum dots as catalysts for CO hydrogenation to methanol.

作者信息

Shi Yuchen, Su Weiguang, Wei Xinyu, Bai Yonghui, Song Xudong, Lv Peng, Wang Jiaofei, Yu Guangsuo

机构信息

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China; College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China.

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China; College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China.

出版信息

J Colloid Interface Sci. 2023 Apr 15;636:141-152. doi: 10.1016/j.jcis.2023.01.008. Epub 2023 Jan 5.

Abstract

CO hydrogenation coupled with renewable energy to produce methanol is of great interest. Carbon coated InO hollow tube catalysts embedded with ultra-low content ZnO quantum dots (QDs) were synthesized for CO hydrogenation to methanol. ZnO-InO-II catalyst had the highest CO and H adsorption capacity, which demonstrated the highest methanol formation rate. When CO conversion was 8.9%, methanol selectivity still exceeded 86% at 3.0 MPa and 320 °C, and STY of methanol reached 0.98 ghg at 350 °C. The ZnO/InO QDs heterojunctions were formed at the interface between ZnO and InO(222). The ZnO/InO heterojunctions, as a key structure to promote the CO hydrogenation to methanol, not only enhanced the interaction between ZnO and InO as well as CO adsorption capacity, but also accelerated the electron transfer from In to Zn. ZnO QDs boosted the dissociation and activation of H. The carbon layer coated on InO surface played a role of hydrogen spillover medium, and the dissociated H atoms were transferred to the CO adsorption sites on the InO surface through the carbon layer, promoting the reaction of H atoms with CO more effectively. In addition, the conductivity of carbon enhanced the electron transfer from In to Zn. The combination of the ZnO/InO QDs heterojunctions and carbon layer greatly improved the methanol generation activity.

摘要

将一氧化碳加氢与可再生能源相结合来生产甲醇备受关注。合成了嵌入超低含量氧化锌量子点(QDs)的碳包覆氧化铟空心管催化剂用于一氧化碳加氢制甲醇。ZnO-InO-II催化剂具有最高的一氧化碳和氢气吸附容量,其甲醇生成速率也最高。当一氧化碳转化率为8.9%时,在3.0MPa和320℃下甲醇选择性仍超过86%,在350℃下甲醇时空产率达到0.98g hg。ZnO/InO量子点异质结在ZnO和InO(222)的界面处形成。ZnO/InO异质结作为促进一氧化碳加氢制甲醇的关键结构,不仅增强了ZnO与InO之间的相互作用以及一氧化碳吸附容量,还加速了电子从In向Zn的转移。ZnO量子点促进了氢气的解离和活化。包覆在InO表面的碳层起到了氢溢流介质的作用,解离的氢原子通过碳层转移到InO表面的一氧化碳吸附位点,更有效地促进了氢原子与一氧化碳的反应。此外,碳的导电性增强了电子从In向Zn的转移。ZnO/InO量子点异质结与碳层的结合极大地提高了甲醇生成活性。

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