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用于高效气态单质汞捕集的具有富硫界面的可控无序硫化铜

Controllable Disordered Copper Sulfide with a Sulfur-Rich Interface for High-Performance Gaseous Elemental Mercury Capture.

作者信息

Liu Cao, Xiang Kaisong, Li Junyuan, Liu Hui, Shen Fenghua

机构信息

School of Metallurgy and Environment, Central South University, Changsha 410083, China.

Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution, Changsha 410083, China.

出版信息

Environ Sci Technol. 2022 Oct 4;56(19):13664-13674. doi: 10.1021/acs.est.2c04859. Epub 2022 Sep 26.

Abstract

Copper sulfide (CuS) has received increasing attention as a promising material in gaseous elemental mercury (Hg) capture, yet how to enhance its activity at elevated temperature remains a great challenge for practical application. Herein, simultaneous improvement in the activity and thermal stability of CuS toward Hg capture was successfully achieved for the first time by controlling the crystal growth. CuS with a moderate crystallinity degree of 68.8% showed a disordered structure yet high thermal stability up to 180 °C. Such disordered CuS can maintain its Hg capture activity stable during longtime test at a wide temperature range from 60 to 180 °C and displayed strong resistance to SO (6%) and HO (8%). The significant improvement can be attributed to the synergistic effect of a moderately crystalline nature and a unique sulfur-rich interface. Moderate crystallinity guarantees the thermal stability of CuS and the presence of abundant defects, in which copper vacancy enhances significantly the Hg capture activity. The sulfur-rich interface enables CuS to provide plentiful highly active S sites for Hg adsorption. The interrelation between structure, reactivity, and thermal stability clarified in this work broadens the understanding toward Hg oxidation and adsorption over CuS and provides new insights into the rational design and engineering of advanced environmental materials.

摘要

硫化铜(CuS)作为一种在气态单质汞(Hg)捕集方面颇具潜力的材料,已受到越来越多的关注,然而如何在高温下提高其活性仍是实际应用中的一大挑战。在此,首次通过控制晶体生长成功实现了CuS对Hg捕集活性和热稳定性的同时提升。结晶度为68.8%的中等结晶度CuS呈现出无序结构,但在高达180°C的温度下具有高热稳定性。这种无序的CuS在60至180°C的宽温度范围内进行长时间测试时,能够保持其Hg捕集活性稳定,并对SO(6%)和HO(8%)表现出较强的抗性。这一显著提升可归因于中等结晶性质与独特富硫界面的协同效应。中等结晶度保证了CuS的热稳定性以及大量缺陷的存在,其中铜空位显著增强了Hg捕集活性。富硫界面使CuS能够为Hg吸附提供大量高活性S位点。这项工作中阐明的结构、反应性和热稳定性之间的相互关系拓宽了对CuS上Hg氧化和吸附的理解,并为先进环境材料的合理设计和工程提供了新的见解。

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