期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 21, 页码 7891-7896出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00595
关键词
-
资金
- UC Riverside startup grant
- National Science Foundation (NSF) Division of Chemical, Bioengineering, Environmental, and Transport Systems, Environmental Engineering Program [CBET-1932942]
- U.S. Department of Energy (DOE) Experimental Program to Stimulate Competitive Research (DOE-EPSCoR) [DE-SC0016272]
- NSF Division of Chemistry, Chemical Catalysis Program [CHE-1566106]
- U.S. DOE, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- NSF Major Research Instrumentation Program [CHE-1338173]
- U.S. Department of Energy (DOE) [DE-SC0016272] Funding Source: U.S. Department of Energy (DOE)
This study introduces a hybrid catalyst for reducing aqueous ClO4- into Cl- at room temperature with 1 atm of H-2, showing high turnover number and turnover frequency.
Perchlorate (ClO4-) is a pervasive, harmful, and inert anion on both Earth and Mars. Current technologies for ClO4- reduction entail either harsh conditions or multicomponent enzymatic processes. Herein, we report a heterogeneous (L)Mo-Pd/C catalyst directly prepared from Na2MoO4, a bidentate nitrogen ligand (L), and Pd/C to reduce aqueous ClO4- into Cl- with 1 atm of H-2 at room temperature. A suite of instrument characterizations and probing reactions suggest that the Mo-VI precursor and L at the optimal 1:1 ratio are transformed in situ into oligomeric Mo-IV active sites at the carbon-water interface. For each Mo site, the initial turnover frequency (TOF0) for oxygen atom transfer from ClOx- substrates reached 165 h(-1). The turnover number (TON) reached 3840 after a single batch reduction of 100 mM ClO4-. This study provides a water-compatible, efficient, and robust catalyst to degrade and utilize ClO4- for water purification and space exploration.
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