A supported Au/HZSM-5 catalyst for toluene removal by air plasma catalytic oxidation using the cycled storage-discharge (CSD) mode†

EES catalysis Pub Date : 2024-10-03 DOI:10.1039/D4EY00159A
Amin Zhou, Xiao-Song Li, Jing-Lin Liu, Lan-Bo Di and Ai-Min Zhu
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Abstract

Air plasma catalytic oxidation of toluene (C7H8) with the cycled storage-discharge (CSD) mode is a promising technology for toluene (C7H8) removal. However, the problem of low CO2 selectivity must be solved. In this work, a novel HZSM-5 (HZ) supported Au catalyst (Au/HZ) with ca. 5.7 nm Au nanoparticles was prepared by combining impregnation-ammonia washing and plasma treatment, and adopted for C7H8 removal. Au/HZ displays a large breakthrough capacity and an excellent oxidation ability of C7H8 in dry and wet air plasma. To investigate the mechanism of CO2 selectivity improvement with the Au/HZ catalyst, air plasma catalytic oxidation of gaseous C7H8 and CO, as well as the adsorption of C7H8 and CO on the catalysts were conducted. For plasma-catalytic oxidation of gaseous C7H8 over Au/HZ, the CO2 selectivity is 97.5%, significantly higher than those of HZ (55%) and Ag/HZ (62%). In situ TPD tests indicate that Au/HZ possesses a moderate adsorption strength for CO and C7H8 compared with HZ and Ag/HZ. Meanwhile, plasma oxidation of CO over Au/HZ reaches 100%, which is much higher than those of HZ (15%) and Ag/HZ (24%). Nearly 100% C7H8 conversion and CO2 selectivity of plasma-catalytic oxidation of C7H8 on Au/HZ can be attributed to the moderate adsorption strength of Au/HZ for C7H8 and CO, and very high plasma catalytic activity for CO oxidation.

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一种负载型Au/HZSM-5空气等离子体催化氧化脱甲苯催化剂,采用循环储放(CSD)模式
空气等离子体催化氧化甲苯(C7H8)的循环储放(CSD)模式是一种很有前途的甲苯(C7H8)脱除技术。但是,必须解决低CO2选择性的问题。采用浸渍-氨洗涤和等离子体处理相结合的方法,制备了一种新型的HZSM-5 (HZ)负载型Au催化剂(Au/HZ), Au纳米颗粒约为5.7 nm,并用于C7H8的脱除。Au/HZ在干湿空气等离子体中均表现出较大的突破容量和优异的C7H8氧化能力。为了研究Au/HZ催化剂提高CO2选择性的机理,进行了空气等离子体催化氧化气态C7H8和CO,以及C7H8和CO在催化剂上的吸附。在Au/HZ条件下,等离子体催化氧化气态C7H8的CO2选择性为97.5%,显著高于HZ条件(55%)和Ag/HZ条件(62%)。原位TPD试验表明,与HZ和Ag/HZ相比,Au/HZ对CO和C7H8具有中等的吸附强度。同时,Au/HZ下CO的等离子体氧化率达到100%,远高于HZ(15%)和Ag/HZ(24%)。Au/HZ对C7H8和CO的吸附强度适中,对CO氧化具有很高的等离子体催化活性,因此等离子体催化氧化C7H8在Au/HZ上的C7H8转化率和CO2选择性接近100%。
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