Journal
ADVANCED SUSTAINABLE SYSTEMS
Volume 6, Issue 1, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adsu.202100307
Keywords
electrocatalysis; heterojunctions; nitrogen fixation; photocatalysis; polyoxometalates
Funding
- National Natural Science Foundation of China [21673176]
- Natural Science Foundation of Shaanxi Province [2021JQ-441, 2021JQ-442]
- Natural Science Foundation of Shaanxi Provincial Department of Education [19JK0853]
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Driven by solar power, the synthesis of Ag/PW12/Zr-mTiO(2) composite material using doping and interface engineering principles has led to enhanced nitrogen chemisorption and ammonia production. The Zr-doping improves nitrogen adsorption, while Ag NPs decoration enhances visible light absorption, ultimately achieving high efficiency in nitrogen fixation and ammonia production.
Driven by solar power and derived electricity, ambient photo- and electrochemical nitrogen fixations are considered promising strategies to produce low-concentration NH3/NH4+. Under the principles of doping and interface engineering, a Ag/PW12/Zr-mTiO(2) composite is fabricated in a one-pot synthesis, where zirconium-doped mesoporous TiO2 is co-decorated with silver nanoparticles (Ag NPs, optimal 1 wt%) and phosphotungstic acid (PW12, optimal 10 wt%). Enhanced nitrogen chemisorption is achieved owing to Zr-doping, where the mesoporous structure of Zr-mTiO(2) favors nitrogen mass transfer. Ag NPs decoration leads to visible light absorption. At the interface, PW12 and Ag NPs decelerate the recombination of photo-generated charge carriers. A Z-scheme mechanism is suggested for the hetero-junction, and the surface plasmon resonance effect of Ag NPs is considered in the composite. Consequently, a NH3/NH4+ production rate of 324.2 mu mol g(cat)(-1) h(-1) is achieved in the photo-driven process, together with the structure-reactivity relationship between transient photocurrent intensity and catalytic efficiency. Moreover, constructing Ag/PW12/Zr-mTiO(2) heterojunction introduces a plentitude of active sites for the electrochemical process, together with enhanced charge transfer efficiency at the interface. Hence, an excellent NH3/NH4+ production rate of 55.0 mu g mg(cat)(-1) h(-1) is accomplished at -0.6 V vs RHE. The robustness and superior activity of Ag/PW12/Zr-mTiO(2) in both photo- and electro-driven processes may offer an opportunity for effectively utilizing sunlight.
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