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Controllable Disordered Copper Sulfide with a Sulfur-Rich Interface for High-Performance Gaseous Elemental Mercury Capture
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2022-09-26 , DOI: 10.1021/acs.est.2c04859
Cao Liu 1 , Kaisong Xiang 2, 3 , Junyuan Li 1 , Hui Liu 1, 2 , Fenghua Shen 1, 2
Affiliation  

Copper sulfide (CuS) has received increasing attention as a promising material in gaseous elemental mercury (Hg0) 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 Hg0 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 Hg0 capture activity stable during longtime test at a wide temperature range from 60 to 180 °C and displayed strong resistance to SO2 (6%) and H2O (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 Hg0 capture activity. The sulfur-rich interface enables CuS to provide plentiful highly active Sx2– sites for Hg0 adsorption. The interrelation between structure, reactivity, and thermal stability clarified in this work broadens the understanding toward Hg0 oxidation and adsorption over CuS and provides new insights into the rational design and engineering of advanced environmental materials.

中文翻译:

用于高性能气态元素汞捕获的具有富硫界面的可控无序硫化铜

硫化铜(CuS)作为一种很有前途的气态元素汞(Hg 0 )捕集材料受到越来越多的关注,但如何提高其在高温下的活性仍然是实际应用的一大挑战。在此,通过控制晶体生长,首次成功地同时提高了CuS对Hg 0捕获的活性和热稳定性。中等结晶度为 68.8% 的 CuS 表现出无序结构,但在高达 180 °C 时具有高热稳定性。这种无序的CuS在60~180℃的宽温度范围内长时间测试中能够保持其Hg 0捕获活性稳定,并对SO 2 (6%)和H 2表现出很强的抵抗力。O (8%)。显着改善可归因于适度结晶性质和独特的富硫界面的协同效应。适度的结晶度保证了CuS的热稳定性和大量缺陷的存在,其中铜空位显着增强了Hg 0捕获活性。富含硫的界面使 CuS 能够为 Hg 0吸附提供大量高活性的 S x 2–位点。这项工作阐明的结构、反应性和热稳定性之间的相互关系拓宽了对 CuS 上 Hg 0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。
更新日期:2022-09-26
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