CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Sheng Deng,Xu Han,Ningqing Lv,Xiaochun Yang,Qiyuan Liu,Yonghai Jiang,Yu Yang,Beidou Xi
Despite the widespread use of biochar as a heterogeneous catalyst in AOPs, there is still a need to clarify the activation mechanism of nitrogen-doped biochar on ferrate (Fe(VI)). The Fe(VI) activation was significantly enhanced by the nitrogen-doped biochar synthesized at 800 °C (BC N -800) in this research, resulting in improved degradation of carbamazepine. Characterizations showed that a honeycomb-like pore and channel structure was formed on the inner layer of modified biochar and the SSA and pore volume were increased five and two times respectively as the temperature raised to 800 °C. Numerous indications indicated that the main active oxidizers in the BC N -800/Fe(VI) system were the high Fe species, and subsequent examination unveiled that the incorporation of nitrogen resulted in decreased resistance to charge transfer and enhanced efficiency of electron transfer for the production of high Fe species. DFT calculation illustrated that the SET path in the BC N -800/Fe(VI) system was spontaneous and single-electron oxygen atom transfer was the primary path for generating more highly reactive Fe(V) species. Notably, the BC N -800 remains stable after the organic degradation reaction and the toxicity of the intermediates produced during degradation decreases. This research will not only establish a theoretical foundation for designing eco-friendly catalysts based on biochar but also boost the investigation of biochar's ecological impacts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
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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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 Environmental Chemical Engineering
·
2025
·
IF 7.2
Hao Li,Manling Zhang,Yufeng Jiang,Yi Liu,Wenjun Duan,Di Lang,Wei Du,Zhaofeng Chang,Peng Zhang,Bo Pan
s Biochar exhibited excellent performance in activating persulfate (PS) for the degradation of organic contaminants. However, the role of endogenous metals in the activation of PS needs to be clarified, which will hinder the understanding of the PS activation mechanism by biochar and the design of efficient biochar for PS activation. In this study, biochars were prepared at different temperatures using cellulose, and trace amounts of Fe (0.069 %) and Mn (0.056 %) were incorporated separately or together into biochar to mimic the endogenous metals whose concentrations were consistent with the ones in local corn stalks. Our results demonstrated that a trace amount of Fe could greatly enhance the removal of ofloxacin (OFL) in the C1000-Fe system. Removing metals from biochar via acid-washing did not significantly impact the removal efficiency of OFL. The Raman analysis showed that Fe could increase the defect structures in C1000-Fe, which were converted during the cycling experiments, indicating they participated in the activation of PS. ROS capturing and quenching experiments confirmed that the increased defect structures via Fe in C1000-Fe facilitate the activation of PS to generate superoxide anions (O 2 •− ) and then convert them into singlet oxygen ( 1 O 2 ) for OFL degradation. Our results highlighted that a trace amount of Fe in biochar enhanced its activation of PS for degradation of OFL via altering the carbon structure, not itself as the activation site, which will benefit understanding the role of endogenous metals in the activation of PS.
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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
·
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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 19
·28525-28537
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IF 0
Qiu Rui,Chen Aiyin,Zhang Peng,Tang Xuejiao,Wang Cuiping,Sun Hongwen
Herein, novel catalysts of Fe-containing zeolite-A (Fe/zeolite-A) were synthesized by exchanging iron ions into zeolite-A framework, and short-chain organic acids (SCOAs) were employed as chelating agents. Reactive Brilliant Blue KN-R (KN-R) was used as a model pollutant to evaluate the performance of these catalysts based on the heterogeneous Fenton reaction. The results showed that Fe-OA/3A, which applied zeolite-3A as the supporter and oxalic as the chelating agent, presented the most prominent KN-R decolorization efficiency. Under the initial pH of 2.5, 0.4 mM KN-R could be totally decolorized within 20 min. However, the mineralization efficiency of KN-R was only 58.2%. Therefore, anthraquinone dyes were introduced to modify zeolite-3A. As a result, the mineralization efficiency of KN-R was elevated to 92.7% when using Alizarin Violet (AV) as the modifier. Moreover, the modified catalysts exhibited excellent stability, the KN-R decolorization efficiency could be maintained above 95.0% within 20 min after operating for nine cycles. The mechanism revealed that the Fe(II)/Fe(III) cycle was accelerated by AV-modified catalyst thus prompting the KN-R decolorization in Fenton-like system. These findings provide new insights for preparing catalysts with excellent activity and stability for dye wastewater treatment.
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Advanced Energy Materials
·
2023
·Vol. 13
·期 27
·2300746
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IF 27.8
Yaoshen Niu,Zilin Hu,Bo Zhang,Dongdong Xiao,Huican Mao,Lin Zhou,Feixiang Ding,Yuan Liu,Yang Yang,Juping Xu,Wen Yin,Nian Zhang,Zhiwei Li,Xiqian Yu,Hao Hu,Yaxiang Lu,Xiaohui Rong,Ju Li,Yong-Sheng Hu
Na-ion batteries (NIBs) are promising for grid-scale energy storage applications. However, the lack of Co, Ni-free cathode materials has made them less cost-effective. In this work, Mg 2+ is successfully utilized to activate the oxygen redox reaction in earth-abundant Fe/Mn-based layered cathodes to achieve reversible hybrid anionic and cationic redox capacities. A high first charge capacity of ≈210 mAh g −1 with balanced charge–discharge efficiency is achieved without O-loss, showing a promising energy cost of $2.02 kWh −1 . Full cell against hard carbon anode without pre-sodiation shows energy density exceeding ≈280 Wh kg −1 with a decent capacity retention of 85.6% after 100 cycles. A comprehensive analysis of the charge compensation mechanisms and structural evolution is conducted. Voltage and capacity loss resulting from partially reversible Fe 3+ migration to the Na layer is confirmed, shedding light on further improvements for low-cost NIB cathodes in application scenarios.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Zhanhong Zhao,He Zeng,Yi Zhou,Mingliang Yuan,Xinghua Chang
To address the inherent contradiction between adsorption/desorption energy barriers of intermediates in single-metal urea oxidation reaction (UOR) catalysts, this study developed a cyanide-bridged bimetallic catalyst , Ni 2 Fe(CN) 6 , via liquid-phase synthesis and plasma modification. Plasma modification enhances the structural stability of the three-dimensional framework and optimizes its electronic properties through selective metal ion substitution and framework reconstruction. In situ electrochemical Raman spectroscopy confirms that the cyanide bridge serves as an electron transport bridge, effectively linking Ni and Fe active centers and providing a stable electron transfer pathway for the Ni³ ⁺/Ni²⁺ redox cycle, leading to a 2.05-fold increase in cycling efficiency compared to untreated catalysts. Benefiting from the synergistic effect of the bimetallic centers, Ni 2 Fe(CN) 6 exhibits superior UOR electrocatalytic performance, achieving an overpotential of only 0.425 V（vs. Hg/HgO） at 10 mA cm −2 . Furthermore, theoretical calculations indicate that the protonation state of amino groups significantly influences the rate-determining step by modulating the reaction pathway. The presence of functionally distinct and diversified active sites enables a multi-pathway synergistic catalytic mechanism, effectively promoting key reaction steps, including amino proton transfer , C-N bond cleavage, and N-N coupling.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
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IF 11.3
Zulqarnain Haider Khan,Han Yu,Hui Li,Syed Shabi Ul Hassan Kazmi,Ruixia Han,Muhammad Azeem,Xin Sun,Zia Ur Rehman,Gang Li
Reactive oxygen species (ROS) are critical mediators of soil biogeochemical processes. While the production of ROS with biochar (BC) in the rhizosphere has not been explored. We demonstrate that BC and Fe-modified biochar (FeBC), prepared at 400°C and 600°C, influence ROS generation in paddy soil containing biodegradable (polybutylene succinate: PBS) and conventional (polystyrene) microplastics (MPs). FeBC, particularly FeBC prepared at 600°C, enhance ROS (O 2 •− , H 2 O 2 , • OH) production in paddy soil. The results of rhizosphere-focused pot experiment simulating field-like flooded conditions highlight that FeBC significantly increased O 2 •− , H 2 O 2 , • OH concentrations, especially with PBS (25.63, 27.69, 35.82 µM/kg, respectively) surpassing control by 3.1–3.6-folds. Iron plaque formation, water-soluble phenols, and microbial activity further influenced ROS dynamics and accelerated MP degradation via oxidative fragmentation (SEM surface fissures), dissolved organic carbon release (484 mg/kg), and SUVA 254 decline (4.6 folds). Microbial shifts toward Actinobacteria (37–43 %) and Firmicutes (25–28 %) correlated with ROS dynamics, linking biotic-abiotic degradation pathways. This work reveals the novel role of FeBC in rhizosphere ROS generation and the environmental behavior of MPs in BC-treated agricultural systems.
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ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Jiahang Liu,Yingying Chu,Xiaoyang Li,Mengying Qian,Weiming Zhang
The co-catalytic effect of hydroquinone/quinone electron shuttle has received great attention in the area of Fenton-like reaction. However, the crucial roles of phenolic or hydroquinone moieties in the chemical structures of organic pollutants have always been overlooked. In this study, we discovered that the introduction of rifampicin (RIF), a representative of rifamycin antibiotics, could trigger complete degradation of atrazine (ATZ) in the Fe(III)/H 2 O 2 system. By exploring the influences of initial Fe(III), H 2 O 2 , RIF concentrations and pH values on ATZ degradation efficiency, key components affecting metal ion valence transitions in the system were identified. Quenching experiments, probe tests and EPR analysis verified that •OH served as the primary active species, while HO 2 •/O 2 •− was also generated. Through monitoring Fe(II) concentration variations and employing mass spectrometric analyses, the oxidation pathway of RIF was elucidated: When mixed with Fe(III), the naphthohydroquinone moiety of RIF immediately acted as a direct electron donor to reduce Fe(III) to Fe(II), while itself being oxidized to RIF-Q. Upon H 2 O 2 addition, it rapidly triggered the classical Fenton reaction with Fe(II) to generate •OH, enabling ATZ degradation. Simultaneously, RIF-Q underwent further oxidative breakdown, with some degradation products retaining the capacity to continuously donate electrons to Fe(III), thereby promoting its reduction. This study provides new insights for the co-catalytic effect of pollutant-derived electron shuttles on the transition of metal ion valences.
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Journal of Energy Storage
·
2025
·
IF 9.8
Sikai Zhang,Rui Yin,Zhilong Tan,Minghai Zhao,Peng Zhou,Pei He,Runjing Zhang,Ziyan Wang,ZhiFeng Huang,Hai Hu,Li Liu
The mixed phosphate Na₄Fe₃(PO₄)₂(P₂O₇) (NFPP) via synergistic coordination of mixed [PO₄]/[P₂O₇] anion groups achieves a flat voltage plateau at 3.2 V (vs. Na + /Na) and a theoretical specific capacity of 129 mAh g −1 , but its practical application is still limited by its inherent low electronic conductivity. Through structural integration of polyanion-type cathode materials, this study innovatively designed and constructed hierarchical Na₄Fe₃(PO₄)₂(P₂O₇)@C mesoporous microspheres (NFPP@CMMS). The NFPP nanocrystals uniformly embedded in a three-dimensional interconnected meso porous carbon matrix (pore size distribution: 2–5 nm). Such hierarchical meso/micro-nano architectures provided expansive ion-exchange interfaces, accelerating Na + de/intercalation kinetics while enhancing electronic conductivity and mitigating structural collapse during cycling. Consequently, the NFPP@CMMS delivers exceptional reversible discharge capacity (121 mAh g −1 at 0.1C), outstanding rate capability (72 mAh g −1 at 50C), and superior cycling stability (90.70 % capacity retention after 3500 cycles at 5C). This triple-synergy strategy—combining nano-confinement effects, interconnected mesoporous channels, and carbon-encapsulated network—provides a novel pathway for developing practical sodium-ion battery cathodes.
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