Cu-ZnO/SrTiO3材料的CO2多碳转化机理及双界面金属调制的光热催化

IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL
Zhiqiang Sun , Shuangjiao Li , Yishun Du , Xiaohu Wu , Hongmei Ma , Haijuan Zhan , Shengping Wang
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引用次数: 0

摘要

在光热条件下,由于C-C耦合过程中需要突破高能量势垒、电子传递效率低以及反应中间体的不稳定性,将CO2高效转化为高能量密度、高附加值的多碳产物(C2+)已成为一项重大挑战。本文提出了界面-金属双调制策略来调制具有强界面效应的Cu-ZnO/SrTiO3光热催化材料,制备的催化剂在光热催化CO2转化过程中C2H6产率为1.55 mmol·g−1·h−1,连续运行50 h后仍保持活性。结果表明,界面与金属共催化剂之间的共调制增强了金属氧化物与载体之间的电子相互作用,并在界面处形成界面态,从而有效地调制了SrTiO3的能带结构,催化剂的带隙值显著降低。同时,光生电子-空穴对的分离效率和多电子的定向迁移都得到了显著提高。此外,CO2- tpd和原位红外等测试证实,这种有效的双调制降低了C-C偶联的能垒,为催化剂提供了更多的活性位点,有利于光热催化CO2向多碳方向还原。本研究为实现在光热催化体系中更有效地将CO2转化为多碳产物以及合理设计催化剂提供了新的思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The photothermal catalysis of the CO2 multicarbon conversion mechanism and dual interface-metal modulation of Cu-ZnO/SrTiO3 materials
Under photothermal conditions, the efficient conversion of CO2 into high energy density and high value-added multi-carbon products (C2+) has become a major challenge due to the high energy barrier that needs to be broken through in the C-C coupling process, the low efficiency of electron transfer and the instability of the reaction intermediate. In this paper, an interfacial-metal dual modulation strategy is proposed for the modulation of Cu-ZnO/SrTiO3 photothermal catalytic materials constructed with strong interfacial effects, and the prepared catalysts exhibit a C2H6 production rate of 1.55 mmol·g−1·h−1 during photothermal-catalyzed CO2 conversion, and the activity is still kept after 50 h of continuous operation. The results showed that the co-modulation between the interface and the metal co-catalysts enhanced the electronic interactions between the metal oxides and the carriers and formed interfacial states at the interface, thus effectively modulating the energy band structure of SrTiO3, and the band gap value of the catalysts was significantly reduced. Meanwhile, the separation efficiency of photogenerated electron-hole pairs and the directional migration of multiple electrons of the catalysts were significantly improved. In addition, tests such as CO2-TPD and in situ infrared confirmed that more active sites were provided for the catalysts, and the energy barrier of C-C coupling was lowered by this effective dual modulation, which was favorable for the photothermal catalysis of CO2 reduction toward the multicarbon direction. The present study provides new ideas for realizing how to convert CO2 into multicarbon products more efficiently in a photothermal catalysis system and the rational design of catalysts.
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来源期刊
CiteScore
8.70
自引率
9.60%
发文量
2421
审稿时长
56 days
期刊介绍: Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.
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