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Construct electron transport path through NH2-MIL-125 modified Fe-doped W18O49 nanowires to enhance photocatalytic nitrogen fixation performance

Journal 2023 · IF 6.2 · 发表于 2023 年 11 月 25 日
作者: Zhenhua Hou,Libo Wang,Gang Liu,Ya Wang,Yuhan Wang,Yangyang Zhang,Xiayu Wu,Nan Li
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摘要

Ammonia has important application value in agriculture and industry as a raw material for producing nitrogen fertilizers and organic chemicals. The Haber-Bosch method is generally utilized to synthesize ammonia through N 2 and H 2 as raw materials in industry, but the process generates serious energy consumption and pollution. In the paper, a heterojunction catalyst is constructed that adopts NH 2 -MIL-125 and Fe-doped W 18 O 49 (Fe-W 18 O 49 ) for photocatalytic nitrogen fixation. Fe-W 18 O 49 is a nanowire containing oxygen vacancies (OVs). OVs can provide active sites for the adsorption and activation of nitrogen gas. The 3D plate-like morphology of NH 2 -MIL-125 can observably reduce the occurrence of nanowires aggregation. This phenomenon can be attributed to NH 2 -MIL-125 playing a supporting role in the fixation of nanowires. New mesoporous are formed between NH 2 -MIL-125 and Fe-W 18 O 49 in the constructed compound catalyst, which can realize efficient mass transfer between the inside and outside of the catalyst. EPR characterization discovers that Fe-W 18 O 49 /NH 2 -MIL-125 cannot produce •O 2 ˗ and •OH radicals. The type II heterojunction forms between Fe-W 18 O 49 and NH 2 -MIL-125. The heterojunction improves the carrier migration path, and the photocurrent intensity is significantly increased. Under simulated sunlight, Fe-W 18 O 49 /NH 2 -MIL-125–2 emerges the best catalytic performance with an ammonia formation rate of 128.2 µmol g −1 h −1 . The yield of ammonia is boosted in comparing with NH 2 -MIL-125 (13 times) and Fe-W 18 O 49 (1.7 times). After several cycles, Fe-W 18 O 49 /NH 2 -MIL-125 remain maintains good stability during the catalytic process. This paper provides a possibility for constructing low-cost heterojunction catalysts in the territory of photocatalytic nitrogen fixation.

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