Confining Free Radicals in Close Vicinity to Contaminants Enables Ultrafast Fenton-like Processes in the Interspacing of MoS2 Membranes

被引:569
作者
Chen, Yu [1 ,2 ,3 ]
Zhang, Gong [3 ]
Liu, Huijuan [3 ]
Qu, Jiuhui [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, Ctr Ecoenvironm Sci, Key Lab Drinking Water Sci & Technol Res, Beijing 100085, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Tsinghua Univ, Sch Environm, Ctr Water & Ecol, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
关键词
confined nanofluids; Fenton-like reactions; membranes; MoS2; nanosheets; reactive oxygen species; HYDROGEN EVOLUTION REACTION; LAMELLAR MEMBRANE; SULFUR VACANCIES; PHASE-TRANSITION; RATIONAL DESIGN; PEROXYMONOSULFATE; NANOSHEETS; DEGRADATION; PERFORMANCE; EFFICIENCY;
D O I
10.1002/anie.201903531
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Heterogenous Fenton-like reactions are frequently proposed for treating persistent pollutants through the generation of reactive radicals. Despite great efforts to optimize catalyst activity, their broad application in practical settings has been restricted by the low efficiency of hydrogen peroxide or persulfate decomposition as well as ultrafast self-quenching of the activated radicals. Theoretical calculations predicted that two-dimensional (2D) metallic 1T phase MoS2 materials with exposed (001) surfaces and (100) edges should have remarkable affinity towards crucial intermediates in the peroxymonosulfate (PMS) activation process. X-ray photoelectron spectroscopy and in situ Raman spectroscopy were used to show that the exposed metallic Mo sites accelerate the rate-limiting step of electron transfer. A lamellar membrane made from a stack of 2D MoS2 with tunable interspacing was then designed as the catalyst. The non-linear transport between the MoS2 nanolayers leads to high water diffusivity so that the short-lived reactive radicals efficiently oxidize contaminants.
引用
收藏
页码:8134 / 8138
页数:5
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