INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yuanliang Yuan,Yisheng Yang,Hongxuan Xie,Xiaocong Zhong,Ruixiang Wang,Zhifeng Xu
Due to their distinctive electronic configuration, transition metal phosphides (TMPs) display remarkable catalytic ability in both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Several strategies have been proposed to increase the catalytic efficiency of TMPs, including heteroatom doping, morphology design, and interface engineering. In this study, CoP hollow nanoflower clusters doped with trace amounts of Fe (Fe–CoP nanoFC) were synthesized via a template-based hydrothermal reaction and high-temperature phosphatization. Compared with those of Fe 2 P and CoP, the OER and HER overpotentials (@10 mA cm −2 ) of the Fe–CoP nanoFC in alkaline solution (pH = 14) were 269 mV and 203 mV, respectively, outperforming those of commercial RuO 2 (326 mV) and 20% Pt/C (221 mV). The overall water electrolysis voltage with the Fe–CoP nanoFC as both HER and OER catalysts was 1.671 V (@10 mA cm −2 ), outperforming the 1.736 V achieved with commercialized Pt/C || RuO 2 . Furthermore, the voltage remained stable during the 14 h of galvanostatic water electrolysis, indicating the potential for long-term stability. Trace Fe doping facilitates the construction of abundant Fe 2 P/CoP heterojunctions, effectively modulates the charge distribution at the interface, and consequently enhances the OER/HER catalytic efficiency of CoP nanoFCs. DFT calculations indicate that the CoP/Fe 2 P heterojunction interface has a higher d-band center and greater local charge density. These properties increase the adsorption strength of OH∗, O∗ and OOH∗, reduce the free energy of adsorption of hydrogen atoms and improve the stability of H∗. As a result, the catalysts exhibit considerable catalytic capacity for the OER and HER.
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Chemical Science
·
2025
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IF 7.4
Yecheng Li,Songjie Meng,Zihong Wang,Hehe Zhang,Xin Zhao,Qingshun Nian,Digen Ruan,Lianfeng Zou,Zhansheng Lu,Xiaodi Ren
Fe single atom catalysts (SACs) with high coordination number have emerged as high-performance catalysts for the conversion of CO2 to CO. However, the influence of alkali cation at the catalyst-electrolyte interface has not yet been understood clearly. Here, we investigate the role of the various alkali metal cations (Na+, K+, Rb+) on catalytic CO2 reduction reaction (CO2RR) behavior on high coordination number Fe SACs (FeN5 and FeN6) obtained from a facile hard template method. We find that larger cations can greatly promote CO2RR and such effects are enhanced with increasing cation concentration. Nevertheless, hydrogen evolution side reaction (HER) on co-existing N heteroatom sites will be worsened. This trade-off highlights the importance of manipulating the reactive sites for SACs. From theoretical simulation and in-situ spectroscopy results, we confirm the functioning mechanism of cations on Fe SACs lies in the enhancement of the adsorption of key intermediates through direct coordination and indirect hydrogen bonding effects. With the rationally designed Fe SACs (FeN5) and the electrolyte condition (1 M KOH), our flow cell test demonstrate a maximum Farady efficiency of CO (FECO) of approximately 100% at 100 mA cm-2. This research provides significant insights for future SACs and electrolyte design.
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Materials
·
2024
·Vol. 17
·期 11
·2488
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IF 3.1
Dongmei Zhao,Xinyao Wang,Libin Wang,Jingzhen Wang,Xu Wang,Weipeng Cheng
Antibiotic residues have been found to have potentially harmful effects on ecological and human health. Carbon nitride-based photocatalysts have widely focused on antibiotic photocatalytic degradation. Herein, we prepared Fe-modified g-C3N4nanorod bunches (FCNBs) using chemical vapor co-deposition. Specifically, through the process of calcination, a blend of urea and chlorophyllin sodium iron salt underwent an intriguing transformation, resulting in the integration of Fe into the framework of the g-C3N4nanorod cluster. The resulting photocatalyst exhibited remarkable stability and superior dispersibility. The prepared FCNBs had a unique structure, which was beneficial for increasing light absorption. Furthermore, the Fe species formed a chemical coordination with the g-C3N4matrix, thereby altering the electronic structure of the matrix. This modification facilitated charge transfer, prolonged the carrier lifetime, and enhanced light absorption, all of which significantly increased the photocatalytic activity. The oxytetracycline degradation efficiency of FCNBs was 82.5%, and they demonstrated outstanding stability in cycle trials. This work introduces a promising photocatalyst for the degradation of antibiotics.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yulu Xu,Yu Mei,Yanjun Li,Chenye Fu,Yuantai Li,Yuheng Zhong,Junxi Song,Gang Yang,Shihuai Deng,Xiaohui Lu,Jiali Peng,Bo Lai
The iron-activated periodate (PI) process may be limited by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. Herein, tungsten boride (WB), serving as a co-catalyst, can effectively overcome the inherent drawback of oxidation reactions. The WB/Fe(III)/PI system exhibited different removal efficiencies toward sulfisoxazole (SIZ) under varying PI concentrations. Based on the qualitative and semiquantitative tests, the generation of reactive species changes with various PI concentrations. Specifically, at low PI concentration, Fe(IV), generated via Fe(II)-mediated PI activation following WB-driven Fe(III) reduction, was the primary reactive species responsible for rapid SIZ removal. However, at high PI concentrations, the limited generation of Fe(IV) contributes only marginally to SIZ removal. In situ Raman characterization and electrochemical tests revealed that at high PI concentration, WB could react with PI and Fe(III) to form high-potential metastable intermediates (WB-Fe(III)-PI*), facilitating direct electron transfer pathway (ETP) from the SIZ to PI. Density functional theory (DFT) calculations further confirmed the interactions among WB, Fe(III), and PI. Besides, at low PI concentrations, the WB/Fe(III)/PI system selectively and rapidly oxidized oxygen-transfer-prone pollutants, while at high PI concentrations, it favored sustained oxidation of electron-rich pollutants. Additionally, WB exhibits excellent reusability during cyclic use. This comprehensive investigation deepens insight into PI-based co-catalytic process and offers an efficient strategy for selecting appropriate oxidant concentrations for wastewater treatment.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Meichun Fu,Zhiyu Shao,Yuan Zhang,Qian Zhu,Kuo He,Mengzhu Zhang,Yuzhu Hou,Laiping Fang,Fei Yan,Shuang Zhang,Jianshi Du,Ping’an Ma,Keke Huang,Shouhua Feng
Despite the multiple advantages of high tissue penetration depth, selectivity, and noninvasiveness of photothermal-assisted antitumor synergistic therapy, developing photothermal agents with multifunctional characteristics, desirable tumor therapeutic effects, and biological stability remains a key challenge. Herein, an electronic structure-regulated strategy is proposed to activate self-adaptive Sn–Fe electron pair centers (Sn2+/Sn4+ and Fe2+/Fe3+) through loading the electron donor Pt (Pt/SFO-1, -2, -3, -4). Experimental and theoretical calculations indicate that abundant dynamic active centers can facilitate the production of reactive oxygen species (ROS), which enables Pt/SFO samples to possess catalase (CAT), peroxidase (POD), and oxidase (OXD) enzyme-like activities. Upon near-infrared (NIR) laser irradiation, Pt/SFO-2 with a Pt load of 0.9% achieves the highest ROS production, showing a 9-fold compared with SnFe2O4 and implements the synergistic therapy of photothermal therapy (PTT), photodynamic therapy (PDT), and chemodynamic therapy (CDT). The electronic state regulation of inorganic photothermal agents not only improves tumor therapeutic effects but also offers a novel strategy to regulate the electron structure of active centers.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yi Fan,Jirui Song,Yongyou Su,Yun Luo,Le Tian,Qingfeng Liu,Zitong Fei,Chenchen Li,Qi Meng,Peng Dong,Yingjie Zhang
The widespread utilization of LiFePO 4 (LFP) batteries has rendered the green regeneration of spent LFP cathode materials (SLFP) an urgent priority. Selective lithium extraction strategies have rapidly advanced through enabling simplified yet efficient lithium recycling. However, under acidic conditions, minor Fe dissolution was observed to significantly reduce the structural stability of regenerated LFP materials while exacerbating Li/Fe antisite defects. A novel strategy based on Fe vacancy site-mediated bond energy reinforcement and nucleation regulation was proposed to achieve structural reinforcement and high-efficiency regeneration. Experimental characterization revealed that Li/Fe antisite defects in regenerated materials were reduced from 1.48 % to 0.93 %, with grain size being significantly refined. The regenerated material exhibited a reversible capacity of 150.2 mAh·g −1 at 1C rate, maintaining 94.74 % capacity retention after 500 cycles, while its discharge capacity at 5C rate was elevated by 60 mAh·g −1 . Environmental and economic assessments conducted via the everbatt model demonstrated significant advantages of this strategy.
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JOURNAL OF MEDICINAL CHEMISTRY
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2025
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IF 6.8
Qing-Hua Shen,Long-Bo Yu,Shan-Ming Yao,Zhi-Yuan Li,Qi-Qi Zhang,Peng Wang,Cai-Ping Tan
Metalloenzyme mimics based on small molecules are valuable therapeutic candidates, but there are few reports on their mechanism of action. Inspired by natural enzymes, we designed two Cu–Fe bimetallic multienzyme mimetics (CuFc1 and CuFc2). Due to the coordination of the bimetallic centers, CuFc1 exhibits mimetic activities for multiple enzymes, including peroxidase (POD), catalase (CAT), superoxide dismutase (SOD), and glutathione oxidase (GSHOx). CuFc1 can catalyze cascade reactions from •O2– and H2O2 to O2 and •OH, which leads to a storm of reactive oxygen species and causes cuproptosis and ferroptosis in cancer cells simultaneously. As CuFc1 treatment upregulates the expression of PD-L1, it acts synergistically with the PD-L1 inhibitor (BMS-1) to remodel the tumor immune microenvironments and stimulates intense anticancer immune responses in vivo. In summary, through reasonable molecular design, we first demonstrate the enormous potential of metallo small molecule-based multienzyme mimics in cancer immunotherapy.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
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IF 6.3
Yuan Ma,Chunhong Li,Muhammad Aizaz Ud Din,Lan Zhao,Nengcong Pan,Yuhan Lei,Nanpu Cheng
Affordable and highly effective electrocatalysts are essential for achieving industrial-scale hydrogenation of water applications. The successful fabrication of Fe-doped CoSe 2 nanosheets supported on nickel foam (Fe x -CoSe 2 /NF) via a two-step electrochemical deposition method is presented in this study, showing their effectiveness as an electrocatalyst for the oxygen evolution reaction (OER) in water splitting. The performance of Fe x -CoSe 2 /NF initially improves with increasing x, reaching an optimal value before subsequently declining. The ideal catalyst, Fe 0.75 -CoSe 2 /NF, requires a low overpotential of 256 mV at 10 mA cm −2 , and even at 100 mA cm −2 , the overpotential remains as low as 291 mV. The catalyst also displays a low Tafel slope of 34.37 mV dec −1 , highlighting the fast OER kinetics. Furthermore, Fe 0.75 -CoSe 2 /NF demonstrates exceptional electrochemical stability. The enhanced OER catalytic performance of Fe-doped CoSe 2, compared to intrinsic CoSe 2, is attributed to the thinner nanosheets structure and optimized electronic structures, which provide a higher density of active sites and facilitate a new reaction coordination with a lower energy barrier during the OER process. These findings not only offer new mechanistic insights into Fe-doped CoSe 2 systems but also provide a scalable and cost-effective pathway for designing next-generation, non-precious-metal-based electrocatalysts.
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COMPOSITES PART B-ENGINEERING
·
2025
·
IF 14.2
Xusheng Chen,Ye Yang,Lina Si,Hongjuan Yan,Zhaoliang Dou,Fengbin Liu,Huanxiong Xia
To address the inadequate bonding strength between machined carbon fiber reinforced polymer (CFRP) and metal, this study investigates a novel precoating treatment utilizing organic nanoparticles. Leveraging the synergistic effect between the silane coupling agent (3-aminopropyl) triethoxysilane (APS) and polydopamine-chelated iron nanoparticles (PDA-Fe), a dense protective layer forms on the damaged CFRP surface. Single lap shear (SLS) tests demonstrated a significant 93 % increase in shear strength for joints with APS-(PDA-Fe) treated CFRP. Comparative studies with inorganic particles—multi-walled carbon nanotubes (MWCNTs), zinc oxide (ZnO), and silica (SiO 2 )—revealed that APS-(PDA-Fe) yielded the highest bonding strength enhancement for milled CFRP. Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), surface wettability analysis, and microscopic morphology characterization elucidated the underlying mechanism: the formation of a protective encapsulating layer that repairs and reinforces damaged fibers, combined with abundant polar functional groups (e.g., hydroxyl, amino, quinone) in APS and PDA-Fe, which substantially enhance resin adhesion to the CFRP surface.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Qifeng Li,Wenzhi Jiang,Xiaoling Wu,Hongming Lou,Xueqing Qiu,Zhixian Li
Single-atom nanozymes (SAzymes) precisely emulate enzyme catalytic centers at the atomic level, offering exceptional catalytic efficiency and selectivity. Inspired by the heme structure of natural enzymes, this study introduces chlorine axial coordination into the Fe–N3O single-atom nanozyme, constructing a unique Fe–N3O–Cl catalytic site (Fe–N/O/Cl–C SA). As a result, the Fe–N/O/Cl–C SA demonstrates remarkable peroxidase-like activity toward the substrate 3,3′,5,5′-tetramethylbenzidine (TMB), achieving a catalytic efficiency 1.96-fold greater than horseradish peroxidase (HRP). Density functional theory (DFT) calculations further reveal that axial chlorine coordination significantly reduces the reaction energy barrier, complementing the planar oxygen coordination, which shortens the activation pathway for H2O2. Moreover, the Fe–N/O/Cl–C SA efficiently catalyzes the oxidative depolymerization of birch lignin under mild conditions, producing high-value aromatic monomers such as vanillin and cinnamaldehyde. These findings underscore the critical role of chlorine axial coordination in enhancing catalytic performance and highlight the great potential of single-atom nanozymes in biomass conversion and renewable energy applications.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Qiansheng Li,Yi Dai,Hong Lu,Xiaoman Li,Fanghao Cheng,Jiti Zhou
Microbial-driven Fenton reactions are essential sources of reactive oxygen species in the aqueous environment and important pathways for pollutant degradation. However, their rates are usually limited by microbial respiration. Herein, N and Fe co-doped CDs (N, Fe-CDs) were used to construct a biological Fenton system with marine community YEP-1 for ketoprofen (KTP) removal. The addition of N, Fe-CDs significantly increased the aerobic degradation rate of KTP by 60.8 % at 48 h. Further analysis showed that N, Fe-CDs enhanced the microbial electron transfer system activity of YEP-1 to produce more H 2 O 2 . Moreover, the regeneration of Fe(II) in extracellular N, Fe-CDs was achieved under aerobic conditions, which was beneficial to activate the extracellular H 2 O 2 for more ·OH generation. Based on the metagenome analysis, N, Fe-CDs significantly increased the populations of genera Exiguobacterium , Leucobacter and Microbacterium . The enriched genes related to electron transfer and Fe(III) reduction were found to be closely associated with Microbacterium . Furthermore, the relative abundances of genes related to the chemotaxis and degradation of aromatic compounds were also increased. These results indicated that biological enzyme-catalyzed processes and N, Fe-CD-mediated Fenton reaction were jointly involved in KTP degradation. This work further advances our understanding of N, Fe-CDs-mediated microbial Fenton reactions.
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MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Ziwei Chen,JinChang Zhao,Qing Li,Rufen Chen,HuiJiao Zhang,Hui Zhao,Kezhong Wu
The synergistic coupling of different metal species endows mixed transition metal oxides (MTMOs) as electrode materials for supercapacitors with multiple redox reaction pathways and enhances the electronic conductivity. In this study, three MoO 2 @FeMoO 4 electrode materials were derived from the precursor PMo 12 @MIL-101(Fe) by pyrolysis at 600 °C, 700 °C, and 800 °C under an O 2 atmosphere. The precursor was composed of polyoxomolybdate (H 3 PMo 12 O 40 , PMo 12 ) and Fe-based metal-organic frameworks (MOFs) MIL-101(Fe). The structural characteristics of the three obtained MoO 2 @FeMoO 4 composites were characterized by XRD, XPS, SEM, and N 2 adsorption measurement. Then, the effects of the pyrolysis preparation temperature for the MoO 2 @FeMoO 4 composites on the energy storage performance of the supercapacitor electrode were evaluated by cyclic voltammetry (CV) and galvanostatic charge/discharge tests. Among three electrodes, the specific capacitance of 339.6 F g −1 of the obtained MoO 2 @FeMoO 4 (700 °C) electrode was the highest compared to 291.2 F g −1 of MoO 2 @FeMoO 4 (600 °C) and 209.7 F g −1 of MoO 2 @FeMoO 4 (800 °C) at a current density of 0.5 A g −1 in 1.0 M NaOH electrolyte. As a result, the different pyrolysis preparation temperatures can alter the atomic microelectronic state and geometric configuration of the MoO 2 @FeMoO 4 , which can construct a high-density Fe–Mo bimetallic multicatalytic active site, thus affecting the activity of the composites. The excellent pseudo-supercapacitance response of the MoO 2 @FeMoO 4 (700 °C) electrode can be ascribed to its larger S BET and greater number of voids, which can generate more Fe–Mo bimetallic active sites and facilitate the electrolyte diffusion, indicating high energy conversion efficiency for potential application in supercapacitors.
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