期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 55, 期 12, 页码 8318-8328出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c01131
关键词
single-atom catalysts; organic pollutant oxidation; electronic polarization; PMS reduction and oxidation; electron migration
资金
- National Natural Science Foundation of China [51808142, 51838005, 51701201]
- introduced innovative R&D team project under the The Pearl River Talent Recruitment Program of Guangdong Province [2019ZT08L387]
- National Key Research and Development Plan [2016YFA0203200]
- DNL Cooperation Fund, CAS [DNL201903]
Single-atom iron catalyst prepared via a cascade anchoring method exhibits exceptional catalytic activity in peroxymonosulfate (PMS) conversion for organic pollutant oxidation, with the high-activity origin attributed to the Fe-pyridinic N-4 moiety that significantly increases active sites for PMS activation.
Single-atom catalysts (SACs) have emerged as efficient materials in the elimination of aqueous organic contaminants; however, the origin of high activity of SACs still remains elusive. Herein, we identify an 8.1-fold catalytic specific activity (reaction rate constant normalized to catalyst's specific surface area and dosage) enhancement that can be fulfilled with a single-atom iron catalyst (SA-Fe-NC) prepared via a cascade anchoring method compared to the iron nanoparticle-loaded catalyst, resulting in one of the most active currently known catalysts in peroxymonosulfate (PMS) conversion for organic pollutant oxidation. Experimental data and theoretical results unraveled that the high-activity origin of the SA-Fe-NC stems from the Fe-pyridinic N-4 moiety, which dramatically increases active sites by not only creating the electronrich Fe single atom as the catalytic site but also producing electron- poor carbon atoms neighboring pyridinic N as binding sites for PMS activation including synchronous PMS reduction and oxidation together with dissolved oxygen reduction. Moreover, the SA-Fe-NC exhibits excellent stability and applicability to realistic industrial wastewater remediation. This work offers a novel yet reasonable interpretation for why a small amount of iron in the SA-Fe-NC can deliver extremely superior specific activity in PMS activation and develops a promising catalytic oxidation system toward actual environmental cleanup.
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