ACS Applied Materials & Interfaces
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2024
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IF 8.3
Binghong Wu,Baoqian Yang,Xinru Wu,Dong-Hau Kuo,Zhengjie Su,Longyan Chen,Pengkun Zhang,Mengistu Tadesse Mosisa,Dongfang Lu,Zhanhui Yuan,Jinguo Lin,Xiaoyun Chen
Nitrogen fixation reaction via photocatalysis offers a green and promising strategy for renewable NH3 synthesis, and catalysts with high-efficiency photocatalytic properties are essential to the process. Herein, we demonstrate a W-doped Sb2OS2 bimetal oxysulfide catalyst (labeled as SbWOS) with abundant oxygen vacancies, heterovalent metal states, and hydrophilic surfaces for nitrogen photoreduction to ammonia. The SbWOS-3 with suitable W-doping exhibited excellent nitrogen fixation activity of 408.08 μmol·g–1·h–1 and an apparent quantum efficiency (AQE) of 1.88% at 420 nm and a solar-to-ammonia (STA) conversion efficiency of 0.082% in pure water under AM1.5G light irradiation. The W-doping not only transforms hydrophobic Sb2OS2 into a hydrophilic catalyst, making it easier for H2O molecules adsorbed on the SbWOS surface and catalyzed into protons, but also endows the SbWOS catalyst with rich oxygen vacancies, acting as the active sites for trapping and activating the N2 molecule, and for trapping and activating H2O to produce the protons for the N2 photocatalytic reduction reaction. The hydrazine drives the SbWOS catalyst with the heterovalent metal states, which acts as the photogenerate electrons quickly hopping between W5+ and W6+ to transfer for the N2 reduction reaction. This study provides a feasible scheme for applying oxygen vacancy defects, heterovalent metal states, and surface hydrophobic-to-hydrophilic wetting engineering in bimetal oxysulfide for N2 photoreduction to ammonia.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Energy
·
2025
·
IF 8.6
Binghong Wu,Xinru Wu,Dong-Hau Kuo,Xiao Tang,Xin Mao,Baoqian Yang,Zhengjie Su,Pengkun Zhang,Longyan Chen,Minhao Liu,Jinguo Lin,Xiaoyun Chen
To reveal the role of bi-vacancy defects and heterovalent states in oxysulfide catalysts for enhancing the photocatalytic hydrogen evolution reaction (PHER), we demonstrate a Br/W co-doped Zn(O,S) catalyst (labeled as Br/W-ZnOS) featuring abundant anionic oxygen vacancies (V O )/cationic zinc vacancies (V Zn ) bi-defects and heterovalent W 5+ /W 6+ states via a facile hydrolysis method. The co-doping of Br and W induces lattice distortions that enable neighboring atoms to leave the lattice, creating surfaces enriched with anionic V O and cationic V Zn defects. The synergistic effect between dual defects forms an efficient electron-hole separation system, enhancing the efficiency of electron-hole pair separation. Density functional theory calculation (DFT) demonstrates that the combination of Br/W co-doping and vacancies significantly reduces the water dissociation barrier and optimizes the surface ∗H generation rate of the photocatalyst. Thus, Br/W-ZnOS exhibits a PHER rate of 3415.7 μmol h −1 , which is 12.5 times higher than the undoped Zn(O,S) catalyst, and achieves an apparent quantum yield (AQY) of 15.41 % at 365 nm, while maintaining good stability with a PHER activity of 3288.1 μmol h −1 after five repeated cycles. This research provides a promising strategy for designing oxysulfide catalysts with synergistically engineered defects for efficient PHER.
研究领域:
材料科学
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催化化学
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理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Sustainable Systems
·
2024
·Vol. 8
·期 12
·2400429
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IF 6.5
Baoqian Yang,Xinru Wu,Zhengjie Su,Benjamin Kunkadma Insua,Pengkun Zhang,Dong-Hau Kuo,Lulu Gao,Xinde Bao,Dongfang Lu,Jinguo Lin,Xiaoyun Chen
V/S co-doped SnO 2 bimetal sulfur-oxides catalysts labeled as (Sn,V) 1- x (S,O) 2- y or (SnVSO) with heterovalent state and oxygen vacancy defect are prepared via a green and facile method. The presence of SnVSO in the heterovalent states of Sn 4+ /Sn 2+ and V 5+ /V 4+ facilitates the rapid transfer of the electrons. It improves the electronic charge lifetime, accelerating the efficiency of the catalytic reduction of pollutants. The V/S co-doped SnO 2 regulates the bandgap energy structure. The hydrazine adjusts the heterovalent metal states to reduce Sn 4+ to Sn 2+ and V 5+ to V 4+ . Also, it introduces oxygen vacancies to SnVSO to maintain the charge equilibrium and increase the active surface reactive sites, which enhance the catalytic activity. The SnVSO-3 prepared with 0.4 mL hydrazine exhibits excellent catalytic activity, which wholly reduces 20 ppm of 100 mL methyl orange (MO), rhodamine B (RhB), methylene blue (MB), hexavalent chromium (Cr 6+ ), and 4-nitrophenol (4-NP) within 6 min. In addition, the SnVSO-3 also has good stability after repeated 6 runs with a reduction efficiency of 96.8%. Therefore, the V/S co-doped SnO 2 sulfur oxide catalysts have a promising potential for reducing Cr 6+ and organic pollutants.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2024
·
IF 10.7
Zhengjie Su,Binghong Wu,Dong-Hau Kuo,Longyan Chen,Pengkun Zhang,Baoqian Yang,Xinru Wu,Dongfang Lu,Jinguo Lin,Xiaoyun Chen
Herein, we demonstrate a Mo/S co-doped BiOBr-based bimetal bismuth sulfur-oxybromide (Mo/S-BiOBr) catalyst with heterovalent molybdenum states and abundant oxygen vacancy defects for photocatalytic hydrogen evolution (PHER) via a facile method. Mo/S co-doping adjusts the energy band structure of BiOBr and expands its visible light absorption. Hydrazine regulates the molybdenum with heterovalent states while endowing Mo/S-BiOBr with oxygen vacancy defects to balance the valence-charge deviations from electrical neutrality induced by Mo6+ → Mo4+. These oxygen-vacancy defects act as active sites for capturing water molecules and activating the H–O–H bond to produce protons for hydrogen generation. The heterovalent Mo6+/Mo4+ states act as photogenerated electron hosts to hop fast between Mo6+ and Mo4+, facilitating efficient electron transfer for the PHER. The hybridization between S 3p and O 2p orbitals improves the stability of continuous PHER. The hydrazine-regulated Mo/S-BiOBr-3 with an optimal n(Mo4+)/n(Mo4+ + Mo6+) ratio and abundant oxygen vacancy defects exhibit an excellent PHER activity of 710.5 μmol h−1 at a catalyst weight of 50 mg and an apparent quantum efficiency (AQE) of 13.9% at 420 nm. After six recycles, the H2 yield of Mo/S-BiOBr-3 decreased by only about 3.5%, indicating its good stability and durability. This work provides a practical approach to using bismuth-based oxyhalides in the PHER.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
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