Filling Mesopores of Conductive Metal–Organic Frameworks with Cu Clusters for Selective Nitrate Reduction to Ammonia
01 natural sciences
0104 chemical sciences
DOI:
10.1021/acsami.2c09241
Publication Date:
2022-07-08T19:09:05Z
AUTHORS (9)
ABSTRACT
The electrocatalytic nitrate reduction reaction (NO3–RR) to ammonia (NH3) under ambient conditions not only has the benefit of lowering energy consumption, but also helps remove contamination. Inspired by unique structure nitrate/nitrite reductase with active spheroproteins encapsulated larger enzymes, herein, we develop an in situ synthetic strategy for construction metal cluster–conductive metal–organic framework (MOF) composite electrocatalysts. metallic Cu clusters are filled into mesopores a conductive copper-based MOF (i.e., CuHHTP); meanwhile, CuHHTP porous provides internal environment limit growth ultrasmall size 1.5 ± 0.2 nm) and restrains their aggregation. obtained Cu@CuHHTP exhibits superb performance NO3–RR. In neutral electrolyte 500 ppm NO3–, shows high NO3– conversion 85.81% selectivity NH3 96.84%. 15N isotope labeling experiments confirm that formation originates from process Theoretical calculations sites electrocatalysts, which proper d-band center "accept–donate" mechanism charge transfer key factors improvement performance.
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