{"title":"基于Fe/Pd双金属串联活性位点的级联催化策略高效去除高纯氯化氢气体中乙炔和乙烯杂质","authors":"Kaihao Li, Yongwang Li, Yang Qin, Zheng Wang, Bingxin Zhu, Yancong Yin, Fumin Wang, Xubin Zhang","doi":"10.1016/j.apcata.2025.120550","DOIUrl":null,"url":null,"abstract":"<div><div>The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a \"stepwise conversion-deep chlorination\" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h<sup>−1</sup>), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120550"},"PeriodicalIF":4.8000,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cascade catalytic strategy based on Fe/Pd bimetallic tandem active sites for efficient removal of acetylene and ethylene impurities from high-purity hydrogen chloride gas\",\"authors\":\"Kaihao Li, Yongwang Li, Yang Qin, Zheng Wang, Bingxin Zhu, Yancong Yin, Fumin Wang, Xubin Zhang\",\"doi\":\"10.1016/j.apcata.2025.120550\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a \\\"stepwise conversion-deep chlorination\\\" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h<sup>−1</sup>), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"708 \",\"pages\":\"Article 120550\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-09-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X2500451X\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X2500451X","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Cascade catalytic strategy based on Fe/Pd bimetallic tandem active sites for efficient removal of acetylene and ethylene impurities from high-purity hydrogen chloride gas
The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a "stepwise conversion-deep chlorination" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h−1), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.