JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Kaizhou Huang,Jiajie Xu,Wei Qu,Tenghui Jin,Yi Yang,Xiao Liu,Rajasekhar Balasubramanian,J. Paul Chen
A hierarchically structured photocatalyst composite bead (CS-PG 0.5% -Fe) was developed in this study through a synergistic electronic modulation strategy, incorporating porphyrin-tailored polymeric carbon nitride (C 3 N 4 por), Fe(III) coordination, and polyethylenimine(PEI)-alginate cross-linked matrix to overcome challenges in Fenton-like wastewater treatment. The multi-component architecture was constructed via triple cross-linking treatment, with comprehensive mechanistic analysis employing in-situ characterization, reactive species tracking, and theoretical calculations to reveal the photo-driven H 2 O 2 self-supply and activation processes. PEI acted as an electron pump and proton-relay mediator to enhance C 3 N 4 charge separation, while the cross-linked structure enabled spatially the confined H 2 O 2 activation. With 0.5 % PEI crosslinking identified as the optimal condition in the material fabrication, the composite achieved an exceptionally high H 2 O 2 production rate and rapid atrazine degradation ( k = 0.0234 min −1 ), and efficient Fe 2+ /Fe 3+ cycling with 96.05 % stability after four consecutive cycles. This study demonstrates an effective approach to simultaneously regulate charge separation and reaction pathways in photocatalytic-Fenton-like systems, offering a scalable solution for energy-autonomous water purification with reduced chemical inputs and recyclable catalytic components.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Ming Ruan,Huajing Zhou,Lingxiang Zhao,Tianding Hu,Liang He,Shaoyun Shan
It is feasible to improve the photodegradation efficiency of organic pollutants by metal-organic frameworks (MOF)-based semiconductors via ligand engineering. In this work, three (Fe/Co)-XBDC-based MOFs were synthesized by introducing different ortho-functional groups X (X = –H, –NO 2 , –NH 2 ) next to the carboxyl group of the organic ligand (i.e., terephthalic acid). The analysis focused on the influence mechanism of the adjacent functional group effect of the ligand on the physicochemical properties of the material and the actual photodegradation activity of TC . Multiple pieces of evidences suggested that the differences in electron-induced and photocharge-transfer mechanisms of the above ortho functional groups affect the crystal morphology and photocatalytic activity of FeCo-MOF during pyrolysis . Interestingly, (Fe/Co)–NH 2 BDC exhibited the highest photocatalytic activity under neutral conditions. The results of density functional theory show that the introduction of a strong donor-NH 2 group can enhance light absorption and act as an “electron pump” to supply electrons to the iron center, accelerating the separation and efficient transport of photogenerated carriers on the ligand-metal bridge. In conclusion, this study is a proposal for a strategy of structural regulation for the enhancement of the catalytic activity of (Fe/Co)-MOFs in the photodegradation of TC.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Peiyun Zhou,Guangtong Hai,Gongchi Zhao,Rushuo Li,Xiubing Huang,Yunfeng Lu,Ge Wang
Developing multifunctional electrocatalysts with excellent hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and 5-hydroxymethylfurfural oxidation reaction (HMFOR) activities will contribute to "carbon neutrality". Here, CeO 2 is introduced into the Co 4 N system as an "electron pump" to attract electrons to transfer from Co 4 N to CeO 2 . The interface electronic structure optimization enables Co 4 N@CeO 2 to exhibit excellent HER, OER, and HMFOR performance. Specifically, to deliver 10 mA cm −2 current density, (1) it only requires low overpotentials of 49 and 263 mV for HER and OER in 1.0 M KOH, respectively; (2) it merely needs an ultra-low potential of 1.22 V RHE for HMFOR in 1.0 M KOH + 300 mM HMF, which is 273 mV lower than the required potential in 1.0 M KOH. Theoretical calculation results show that the introduction of CeO 2 effectively reduces the barriers for potential-determining steps of HER and OER, and optimizes OH - adsorption to promote the HMFOR process.
研究领域:
材料科学
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能源化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Bin Wang,Hailong Chen,Fangcheng Huang,Jinyuan Liu,Gaopeng Liu,Yu-Xiang Weng,Yuanbin She,Xingwang Zhu,Huaming Li,Jiexiang Xia,Paul K. Chu
In order to enhance the efficiency of artificial photosynthesis, it is imperative to improve the hysteretic migration and separation efficiency of photogenerated charge carriers. Herein, ultrathin Bi 4 O 5 Br 2 (BOB) nanosheets are prepared vertically and uniformly on the surface of hollow N-doped carbon spheres (NC) to produce a hollow confined nanoreactor (BOB@NC). The graphite layer and N in NC act as a tandem electron pump for the rapid transfer of photogenerated electrons from BOB to the NC surface via the Bi-C bridging bond between BOB and NC, and the electrons on the NC surface continue to move to the N-induced defect energy levels. This NC electron pump facilitates the transfer of the photogenerated electrons in a directional, rapid, and efficient manner. Meanwhile, the adsorption of CO 2 molecules and hydrogenation of *CO to *CHO at the N site on NC are kinetically spontaneous, thereby significantly reducing the CO 2 reduction reaction energy barrier of BOB. As a result, the efficiency of CO 2 hydrogenation reduction to CO and CH 4 by BOB@NC is 3.31 and 11.15 times higher than that by the BOB monomer, respectively. The hollow confined electron pump reactor reveals a novel strategy for the design and fabrication of catalysts for high-performance artificial photosynthesis.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 39
·16131-16143
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IF 6.7
Jingzhi Wang,Mei Li,Zhiliang Jin
Dynamics and morphology play a crucial role in the field of photocatalytic hydrogen production. Regulating the transfer of photogenerated charges is an effective way to improve the catalytic activity. In this paper, 1T-WS2 is introduced into a p–n heterostructure, ZnCdS/NiV-LDH, as a metalloid electron pump to transfer photogenerated electrons from semiconductors with larger work functions to metalloid materials with smaller work functions, effectively to attract photogenerated electrons, and promote charge rearrangement at the p–n heterostructure interface, so as to achieve the best utilization efficiency of photogenerated charges. Second, adjusting the morphology to increase the light absorption area of the catalyst is also a way to improve the photocatalytic activity. Two different nanosheet structures dispersed heavily stacked ZnCdS, increasing the light absorption area of the system. The optimal catalyst ratio achieves a hydrogen evolution rate of 22.37 mmol g−1 h−1, achieving 7.98% AQE and 2.12% STH conversion efficiency at 450 nm. The potential mechanism was demonstrated through in situ XPS. This study provides new insights into adding “electron pumps” to heterostructures to enhance photocatalytic activity.
研究领域:
材料科学
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催化
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纳米技术
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光化学
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产品关联
DOI
PubMed
高影响因子
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