ACS Catalysis
·
2025
·
IF 13.1
Yuyao Yang,Xuan Bie,Xiaoying Qi,Yongqing Xu,Qinghai Li,Yanguo Zhang,Hui Zhou
Aqueous phase reforming of methanol (APRM) offers a method for releasing H2 from the liquid phase, by which H2 can be stored in methanol safely. It is an efficient way to design high-performance catalysts by controlling the hydroxyl (OH) groups, but its mechanism for affecting the APRM is still unclear. Herein, we loaded Pt on three types of Al2O3 (nanopolyhedron, nanosheet, and nanorod Al2O3) with different OH contents and types. Among them, Pt/nanorod Al2O3 exhibited the highest H2 production rate of 20.4 μmol g–1 s–1 with 96.6% H2 selectivity at a low temperature of 190 °C. This was attributed to the roles of hydroxyl groups in modulating Pt states. On nanopolyhedron, nanosheet, and nanorod Al2O3, the bonding of Pt with O atoms became more favorable as the dehydroxylation happened. In particular, on nanorod Al2O3, the dehydroxylation process generated a high density of five-coordinated Al (AlV) sites, facilitating the dispersion and anchoring of Pt particles. Moreover, the special OH groups (hydrogen bond donor) on nanorod Al2O3 promoted Pt particle reduction via the movement of electrons. Ultimately, the results demonstrated the influence of OH groups on the dispersion and reduction of active metals, offering perspectives for designing catalysts for APRM through hydroxyl control.
研究领域:
催化化学
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能源材料科学
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DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Youwei Yang,Jianxing Wang,Yan Gao,Xuekun Tang,Chunying Wang,Xianping Luo
ZnFe 2 O 4 catalysts synthesized via hydrothermal (ZFO-H) and sol-gel (ZFO-S) methods were employed to activate peroxodisulfate (PDS) under UV light for the efficient conversion of low-concentration NH 4 + -N into environmentally benign N 2 , offering a promising solution for advanced wastewater treatment. Characterization revealed that the sol-gel-derived ZFO-S exhibited uniform agglomeration, smooth surfaces, and an 80% reduction in surface hydroxyl density (as indicated by the FTIR peak area at 3320 cm -1 ), outperforming both hydrothermally prepared and commercial ZnFe₂O₄ (ZFO-H and ZFO-M, respectively). This study addresses the critical challenge of ammonia nitrogen removal in wastewater, where conventional methods often struggle with low efficiency or secondary pollution. Mechanistic studies demonstrated that ZnFe 2 O 4 facilitated electron transfer at Zn sites to activate PDS, generating reactive species dominated by singlet oxygen ( 1 O 2 ), which drove NH 4 + -N oxidation. Density functional theory (DFT) calculations further elucidated the reaction pathway, highlighting preferential adsorption of NH 3 at oxygen sites on the ZnFe 2 O 4 (311) surface, followed by sequential dehydrogenation and coupling to form N 2 . Under optimal conditions (pH >9.25, 10 mM PDS, 25°C, 3 h), 97.40% of initial 50 mg/L NH₄ + -N was converted to N₂, with negligible NO 3 − byproduct formation (< 6%), demonstrating high feasibility for practical wastewater remediation. The reduced surface hydroxyl groups and lower work function of ZFO-S enhanced electron transfer, underscoring its superior catalytic activity. This work provides a novel strategy for designing hydroxyl-regulated photocatalysts tailored for wastewater treatment and advances the mechanistic understanding of persulfate-based ammonia nitrogen remediation in engineered water systems.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Liping Lian,Hui Xu,Ruchen Shu,Yujie Tan,Nan Wang,Jinzhu Ma,Feng Qin,Danyan Cen,Jianyuan Hou,Renxi Zhang
A novel catalyst was fabricated using a two-step nonthermal plasma method by regulating surface hydroxyl groups on Na/activated carbon (AC) with 0.1 wt% Pt loading (Pt/Na/AC (P&P)) and achieved high formaldehyde (HCHO) oxidation performance at ambient temperature. Based on characterization results, we found that in the first step of nonthermal plasma treatment under argon–water, the proportion of terminal OH groups (ter-OH groups) evidently increased. Following the introduction of Na and Pt, the relative abundance of doubly bridged OH groups connecting C and Na (briNa–C-OH groups) and Pt2+ species also increased in the second step of nonthermal plasma reduction under argon, resulting in enhanced HCHO catalytic oxidation capability through a rapid reaction pathway ([HCOO−] + [OH]a → CO2 + H2O). Compared with the catalyst prepared via nitric acid oxidation and thermal deposition (Pt/Na/AC (H&T)), more Pt–Ox–Na species and surface OH groups were obtained on the Pt/Na/AC (P&P) catalyst, which not only reduced Pt consumption but also improved HCHO catalytic activity with around 100% conversion of HCHO to CO2 at 25 °C, while the Pt/Na/AC (H&T) catalyst only achieved 70% conversion. This work thus provides a new strategy for HCHO oxidation at room temperature and a novel perspective on the environmentally friendly synthesis of effective noble catalysts.
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 6
·1286
·
IF 4.6
Yiran Zhang,Boyuan Xuan,Jiekai Wang,Xiang Chen,Changwei Zhao,Lixia Zhao,Jing Kang
The rational design of BiOBr photocatalysts with optimized surface properties and enhanced photooxidative capacities is crucial. This study proposes a synergistic strategy combining hydroxyl-rich solvents with polyvinylpyrrolidone (PVP) surfactants to modulate the structural and electronic properties of BiOBr through a solvothermal approach. The resulting self-assembled microspheres demonstrated exceptional efficiency in degrading ciprofloxacin (CIP), methyl orange (MO), and rhodamine B (RhB). Among the synthesized variants, BiOBr-EG-PVP (fabricated with ethylene glycol and PVP) exhibited the highest photocatalytic activity, achieving near-complete removal of 20 mg/L CIP and RhB within 10 min under visible light irradiation, with degradation rates 60.12–101.73 times higher than pristine BiOBr. The structural characterization revealed that ethylene glycol (EG) not only induced the formation of self-assembled microspheres but also introduced abundant surface hydroxyl groups, which simultaneously enhanced the hole-mediated oxidation capabilities. The incorporation of PVP further promoted the development of hierarchical honeycomb-like microspheres and synergistically enhanced both the hydroxyl group density and photooxidative potential through interfacial engineering. Density functional theory (DFT) calculations confirmed that the enhanced photooxidative performance originated from an increased surface oxygen content. This work elucidates the synergistic effects of hydroxyl-rich solvents and surfactant modification in the fabrication of advanced BiOBr-based photocatalysts, providing new insights for high-performance photocatalysis for environmental remediation.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
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