WATER RESEARCH
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2025
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IF 12.4
Haokun Bai,Peike Cao,Lanlan Liang,Shuo Chen,Xie Quan
Metal atomic cluster (AC) catalysts exhibit remarkable catalytic activity in environmental catalysis owing to their tunable structural and electronic properties regulated by electronic metal-support interactions (EMSI). Nevertheless, the precise size control of metal AC remains challenging owing to their inherent aggregation tendency under harsh synthetic conditions. Herein, we propose a confined synthesis strategy for fabricating cobalt AC within the interlayer channels of a two-dimensional molybdenum disulfide membrane (CoAC@MoS 2 membrane) for peroxymonosulfate (PMS) activation. The interlayer confinement of MoS 2 nanosheets enforces the in-plane assembly of metal precursors, yielding ultrafine CoAC (2.1 nm) with excellent Fenton-like activity (0.733 min -1 ), outperforming unconfined Co nanoparticles (29.3 nm, 0.291 min -1 ). Experiments and density functional theory calculations reveal that electrons transfer from sulfur vacancy and Mo sites in MoS 2 to Co 3d orbitals, generating electron-rich Co sites with an upshifted d -band center, which optimizes PMS adsorption and electron transfer to generate SO 4 ⚫- and ⚫OH radicals. The as-prepared CoAC@MoS 2 membrane achieved a sulfamethoxazole degradation rate of 5.33 × 10 6 μmol g metal -1 s -1 , which was 1-2 orders of magnitude higher than state-of-the-art nanoconfined catalytic membranes, and also proved effective in treating secondary pharmaceutical wastewater. This work establishes a universal paradigm for size and electronic structure engineering of metal catalysts through spatial confinement, advancing the development of high-performance Fenton-like catalytic systems for sustainable water remediation.
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DOI
PubMed
高影响因子
Chem
·
2022
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IF 25.832
Tao Liu,Yuxin Chen,Yaming Hao,Jianxiang Wu,Ran Wang,Limin Gu,Xuejing Yang,Qiang Yang,Cheng Lian,Honglai Liu,Ming Gong
The ion-enriched electrode-electrolyte interface is a unique characteristic of electrocatalytic reactions that can effectively tune the local chemical environment. In this study, we discovered a strong synergy between borate and fluoride anions for water oxidation in neutral conditions. Under an optimal ratio of the two anions, the water oxidation current significantly outperforms the individual counterparts by almost an order of magnitude. This synergy was greatly attributed to the hierarchical anions at the interface, with borate approaching the surface and fluoride extending out, as revealed by in situ surface-enhanced Raman spectroscopy and molecular dynamics simulation. This hierarchical anion arrangement created two kinetics regions, with one borate-dominating region to lower the onset potential and one fluoride-dominating region to sustain a larger current. Using the synergized electrolyte, a low-cost and facilely synthesized Co(OH) 2 electrode could achieve an outstanding performance of 100 mA/cm 2 at 1.791 V versus RHE under pH = 7.87 with a 2-week-long durability.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Zimo Lou,Jiang Xu,Jiasheng Zhou,Kunlun Yang,Zhen Cao,Yizhou Li,Yuanli Liu,Liping Lou,Xinhua Xu
Atomic H* has been regarded as the key active species for the electrocatalytic hydrodechlorination (ECH), and the electrode design and operation conditions are related to the atomic H* generation. However, there is limited understanding of how the operation parameters affect the atomic H* generation and utilization. Due to the fact that Pd was inefficient in water dissociation step, MnO 2 was combined with Pd to construct a novel Pd/MnO 2 /Ni foam cathode. Cyclic voltammetry confirmed that Pd/MnO 2 /Ni foam cathode with MnO 2 load of 0.51 mg cm −2 possessed the highest atomic H* generation and ECH activity. Excessive Pd load (>0.44 mg cm −2 ) was detrimental to ECH because of the side hydrogen evolution reaction (HER). Operation conditions (e.g. applied current and electrolyte concentration) would directly affect the cathode potential, which was an important indicator of the atomic H* generation. The optimal cathode potential was determined to be −0.85 V when the applied current was 10 mA in this study. The electrolyte concentration of 10–15 mM was able to provide sufficient atomic H* for ECH, while excessive input of electrolyte would favor HER but inhibit ECH. ECH at acidic and neutral/alkaline solution underwent different pathways for atomic H* generation and further affect the utilization of atomic H*. After 120 min reaction, >70% of atomic H* could be selectively used for ECH at initial pH of 4.0 and 5.0, while only ∼37% was used for ECH at initial pH of 7.0. This work correlated the reactivity of electrode with the atomic H* and cathode potential, which would provide strategies for ECH catalyst design and operation optimization.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Haokun Bai,Lanlan Liang,Shuo Chen,Hongtao Yu,Xie Quan
Herein, the role of nanoconfinement on modulating the electronic structure of the catalyst that influences the efficiency of advanced oxidation processes (AOPs) was investigated. Peroxymonosulfate (PMS)-based AOP was conducted within the nanoconfined sub-nanometer interlayer channels of a 2D NiFe layered double hydroxide membrane (NiFeM). The interlayer-confined NiFeM exhibited complete removal of sulfamethoxazole, with a degradation rate constant of 211.67 s −1 that was 2.6–946.2 times higher than previously reported nanoconfined AOPs systems, and also demonstrated broad pH working range and anti-interference ability with excellent catalytic stability in 25 h. Theoretical calculations suggested such interlayer confinement upshifted the catalyst metal d-band center, accounting for strengthened PMS adsorption and electron transfer from catalyst to PMS molecules. This work embodies the interlayer confinement effect on modulating the electronic structure of catalyst and provides insights for designing catalysts with excellent capability for environmental remediation, energy conversion and chemical synthesis.
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Na Wang,Yibo Zhang,Zelin Meng,Mingyang Song,Heming Zhao,Yang Wang,Shuai Bai,Jianglei Hu,Fengwei Shi,Xia Yang
Addressing the low surface area and high charge recombination of graphitic carbon nitride (g-C 3 N 4 ), this study employs a synergistic carboxylation and MOF-loading strategy. Copper-based MOF (Cu-MOF) was uniformly loaded onto carboxylated spherical g-C 3 N 4 (C 3 N 4 –C) via a solvothermal method, creating a visible-light-responsive C 3 N 4 –C-MOF photocatalyst. Material characterization results indicate that the characteristic peak at 1632 cm −1 in the Fourier Transform Infrared Spectroscopy confirms the successful grafting of 4-carboxybenzoic acid (4-CBA). Carboxylation enhanced hydrophilicity and optimized surface charge, improving reactant adsorption. Photoelectrochemical tests showed significantly boosted visible light absorption, increased photocurrent density, and reduced EIS arc radius, confirming efficient interfacial charge separation. Photocatalytic hydrogen production experiments revealed that under simulated solar irradiation, the hydrogen production rate of C 3 N 4 –C-MOF2.0 reached up to 12.68 mmol g −1 h −1 , representing an approximately 1.68-fold increase compared to the unmodified C 3 N 4 -MOF. This work provides a novel approach for designing MOF/functionalized g-C 3 N 4 composites, advancing solar-driven hydrogen production.
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高影响因子
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