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硫迁移增强核壳 C@MnO 中的质子耦合电子转移以实现高效 CO 脱附

Sulfur Migration Enhanced Proton-Coupled Electron Transfer for Efficient CO Desorption with Core-Shelled C@MnO.

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, PR China.

MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, PR China.

出版信息

Environ Sci Technol. 2024 Mar 12;58(10):4606-4616. doi: 10.1021/acs.est.3c09875. Epub 2024 Mar 1.

Abstract

Transforming hazardous species into active sites by ingenious material design was a promising and positive strategy to improve catalytic reactions in industrial applications. To synergistically address the issue of sluggish CO desorption kinetics and SO-poisoning solvent of amine scrubbing, we propose a novel method for preparing a high-performance core-shell C@MnO catalyst for heterogeneous sulfur migration and in situ reconstruction to active -SOH groups, and thus inducing an enhanced proton-coupled electron transfer (PCET) effect for CO desorption. As anticipated, the rate of CO desorption increases significantly, by 255%, when SO is introduced. On a bench scale, dynamic CO capture experiments reveal that the catalytic regeneration heat duty of SO-poisoned solvent experiences a 32% reduction compared to the blank case, while the durability of the catalyst is confirmed. Thus, the enhanced PCET of C@MnO, facilitated by sulfur migration and simultaneous transformation, effectively improves the SO resistance and regeneration efficiency of amine solvents, providing a novel route for pursuing cost-effective CO capture with an amine solvent.

摘要

通过巧妙的材料设计将有害物种转化为活性位是提高工业应用中催化反应的一种很有前景和积极的策略。为了解决胺洗涤中 CO 解吸动力学缓慢和 SO 中毒溶剂的问题,我们提出了一种新的方法,用于制备高性能核壳 C@MnO 催化剂,用于非均相硫迁移和原位重构活性-SOH 基团,从而诱导增强质子耦合电子转移(PCET)效应,促进 CO 解吸。正如预期的那样,当引入 SO 时,CO 解吸的速率显著增加了 255%。在台架规模上,动态 CO 捕获实验表明,与空白情况相比,SO 中毒溶剂的催化再生热负荷降低了 32%,同时还证实了催化剂的耐久性。因此,通过硫迁移和同时转化促进的 C@MnO 的增强 PCET,有效地提高了胺溶剂的 SO 抗性和再生效率,为采用胺溶剂进行具有成本效益的 CO 捕获提供了一条新途径。

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