CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Qi Chen,Zefeng Yang,Yueling Chen,Jionghua Wu,Jimmy C. Yu,Ling Wu
The fabrication of single atoms on MIL-125(Ti) for photocatalytic ammonia synthesis. • SAs modulate the local electronic structure for charge mobility and separated active site. • The favorable N 2 activation and protons supply optimizes the reduction kinetics. • Magnetic field-induced spin flipping to charge utilization further boost the activity. Photocatalytic nitrogen fixation is an attractive alternative to the energy-intensive traditional ammonia synthesis. However, the major challenge is that most photocatalysts are limited by their low charge mobility, insufficient molecules activation and sluggish reaction kinetics. Herein, we integrated single atoms (Co, Fe, Ni) on MIL-125(Ti) functionalized with sulfhydryl (MIL-125(SH) 2 , MTS) to afford Co-MTS, Fe-MTS and Ni-MTS for photocatalytic nitrogen reduction. Through uniformly dispersed SAs (single atoms) coordinated with O and S atom, such intimate interaction and charge redistribution can efficiently regulate the unsaturated Ti sites for N 2 adsorption and activation. Moreover, the introduced SAs species also serve as separated active center for water oxidation to promote H 2 O adsorption and protons release, kinetically optimizing protons supply and energy barrier of rate rate-determining step for N 2 hydrogeneration. Benefited from the spatially separated metal node-SAs dual sites and favorable reaction energy barrier, the optimized Ni-MTS sample shows an ammonia yield rate of 72.6 μmol·g −1 ·h −1 with an apparent quantum efficiency of 0.49% at 400 nm. This can be further enhanced by magnetic field-induced spin flipping contributed to charge utilization. This work would inspire the development of other high-efficiency single atom/MOFs that combining molecular activation and protons supply for photocatalysis.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
·
IF 4.6
Wenhua Li,Ruilin Wang,Xiang Li,Ge Gao,Chuanyong Yan,Qianqiao Chen
ZIF confinement disperses CoFe nitride uniformly and tunes Co/Fe ratio precisely. • Co/Fe bimetallic coupling lead to synergistic effects for bifunctional HER/OER. • Low overpotentials reach 85 mV (HER@10 mA·cm −2 ) and 273 mV (OER@50 mA·cm −2 ). • Overall water splitting requires 1.59 V at 10 mA·cm −2 with durability over 100 h. CoFe-based materials are considered promising bifunctional catalysts for overall water splitting due to multicomponent synergistic effects. However, unrestricted metal atom migration during high-temperature synthesis causes particle aggregation and excessive Co–Fe interdiffusion, which destroys bimetallic interfacial structures, covers active sites, and hinders electronic modulation, thus limiting catalytic activity and stability. To solve these problems, a ZIF-assisted spatial confinement strategy is adopted herein. The ZIF framework constrains high-temperature atomic migration, alleviates particle coarsening, and weakens metal interdiffusion to maintain intact bimetallic interfacial environments, while exposing sufficient active sites. Further combining carbonization and in-situ nitridation modification, a composite system of CoFe metal nitride and N-doped carbon was prepared, significantly improving the kinetic properties of HER and OER. The optimal catalyst achieves an overpotential of 85 mV for the HER at 10 mA·cm −2 , and 273 mV for the OER at 50 mA·cm −2 , exhibiting superior catalytic performance compared with commercial noble-metal benchmarks. The assembled overall water splitting system requires only 1.59 V at a working current of 10 mA·cm −2 , and can operate stably for 100 h at 50 mA·cm −2 . This work provides a reliable strategy for inhibiting high-temperature structural degradation of CoFe-based catalysts toward high-efficiency and durable electrocatalytic water splitting.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Shanhai Zhao,Yidan Luo,Chunhe Li,Kuankuan Ren,Yanyan Zhu,Weidong Dou
The synthesis of renewable fuel by CO 2 reduction is a promising research direction. The CO 2 reduction reaction may be promoted using photothermal catalysis to achieve efficient CO 2 conversion under mild conditions. In this context, designing efficient catalysts is urgent. In this work, ABO 3 (A = La, Ce; B = Ni, Co, Fe) perovskite catalysts were prepared by coprecipitation and calcination . Experimental results show that the A-site ions and B-site ions in ABO 3 perovskite nanomaterials have a great influence on their structure and photothermal catalytic performance. Among them, the LaNiO 3 catalyst shows excellent photothermal catalytic performance in the conversion of CO 2 to CO and CH 4 , which can generate 0.16 mmol g −1 h −1 CO and 1.38 mmol g −1 h −1 CH 4 at low CO 2 and H 2 concentrations. For the LaNiO 3 sample, its enhancement of catalytic performance mainly benefits from the largest number of active sites, the fastest carrier transport rate, and a relatively suitable band edge position compared with other catalysts. This study proposes a new method for improving the activity and selectivity of photothermal CO 2 reduction and offers a new direction for the recycling of waste gas.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Qian Zhao,Lei Liu,Ying Du,Sisi Jiang,Tingshun Jiang
Rational design of non-noble metal electrocatalyst with high stability and activity for OER is desirable for the production of renewable energy to solve the environmental crisis. Starting from Prussian blue analogues (PBAs) with special advantages, the trimetallic hollow structural Co-Fe-P/Cu 3 P/CF covered with extended nanosheets grown on nanorods was synthesized via ion exchange and calcination approaches in this study. The overpotential of the prepared electrode was only 205 mV at a current density of 100 mA cm − 2 , and it can maintain the stable catalytic activity for at least 60 h. The prominent electric performance is mainly attributed to the construction of the unique morphology, in which the rod-shaped structure can promote the transportation of the reactants, and the hollow structure as well as the nanosheets outside can expand the specific surface area. The electronic interaction between multiple metals can also improve the conductivity of the catalyst. The characterization analysis of the post electrode after long-term oxygen evolution reaction imply that the surface of the catalytic electrode was partially oxidized to the corresponding oxide, which can generate the new active sites to maintain the high catalytic activity together with the residual phosphide. Our research might provide a new reference for the deep exploration of PBA-based materials applied in electrochemical energy conversion and storage.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
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IF 5.2
YuXin Zhao,Jiaxian Liu,Tong Zhang,FangXun Liu,Man Zheng,Kun Shi,JinPeng Liu,Yufan Zhang,Huan Wang
The exploration of an inexpensive catalyst with effective oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) activities to replace precious metal electrocatalysts has been of great interest in recent years. In this paper, CNT@Co-Fe/FePc composites were synthesized with high efficiency using a self-assembly strategy. In the synthesis process, carbon nanotubes (CNTs) were synthesized as the base material using crab shells as templates and honey as the carbon and nitrogen source. CoFe alloy nanoparticles derived from CoFe-based prussian blue analogs were self-assembled and anchored on CNTs, and then iron phthalocyanine with Fe-N 4 portion was coupled with CNTs by π-π stacking. Finally formed a homogeneous and stable composite material. The self-assembly method is simple and efficient to achieve good metal loading. The prepared CNT@Co 2 -Fe 1 /FePc exhibits excellent catalytic performance and stability for OER and ORR in alkaline electrolyte . The overpotential at 10 mA cm −2 of CNT@Co 2 -Fe 1 /FePc for OER is 343 mV with a very small Tafel slope of 43.59 mV dec −1 . CNT@Co 2 -Fe 1 /FePc has high methanol tolerance and persistence for ORR. This work provides a strategy for the construction of transition metal-carbon composite electrocatalytic materials with excellent catalytic performance and stability for OER and ORR reactions.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Zhendong Yu,Jiachen Ma,Jinlan Dai,Shiyu He,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Junfeng Chen,Minghua Liu
In this study, a bimetallic composite catalyst (Co–Fe@C) was fabricated with calcination at high temperature (800 °C) by using Co-MIL-101 (Fe) as the precursor. The characterization results showed that the resulted Co–Fe@C composite mainly consisted of carbon, FeCo alloys, Fe 3 O 4 , Co 3 O 4 and FeO, and owned evident magnetism. In addition, the Co–Fe@C was employed to activate the peroxydisulfate (PDS) to degrade a representative organic pollutant ( p -arsanilic acid, p -ASA) and the main factors were optimized, which involved 0.2 g L −1 of catalyst dosage, 1.0 g L −1 of PDS dosage and 5.0 of initial pH. Under the optimal condition, Co–Fe@C/PDS system could completely degrade p -ASA (20 mg L −1 ) in 5 min. In the Co–Fe@C/PDS system, SO 4 − · , Fe(IV) and ·OH were the main species during p -ASA degradation. Under the attack of these species, p -ASA was first decomposed into phenols and then transformed into the organics acids and finally mineralized into CO 2 and H 2 O through a series of reactions like hydroxylation, dearsenification, deamination and benzene ring opening. Importantly, most of the released inorganic arsenic species (93.40%) could be efficiently adsorbed by the catalyst.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
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IF 5.091
Bin Hu,Jin-Yun Yuan,Jia-Yue Tian,Minghua Wang,Xue Wang,Linghao He,Zhihong Zhang,Zhuo-Wei Wang,Chun-Sen Liu
A new bimetallic Co/Fe-MOF was synthesized and phosphatized to produce a visible-light-active Co/Fe binary metal phosphide embedded in a mesoporous carbon matrix (denoted by CoP/Fe 2 P@mC). The results of X-ray diffraction and photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy reveal the formation of CoP and Fe 2 P nanoparticles together with the Co and Fe metallic state. Combining the high electron–hole separation rate of Fe 2 P@mC, fast electron transfer of CoP@mC, and the strong adsorption of mesoporous carbon, the as-prepared CoP/Fe 2 P@mC catalyst exhibits substantially enhanced photocatalytic activity toward rhodamine B (RhB) degradation under visible light irradiation. Visible light harvesting efficiency is enhanced by the suitable bandgap structure of the CoP/Fe 2 P@mC photocatalyst. Moreover, the possible photocatalytic mechanism of CoP/Fe 2 P@mC toward RhB degradation was proposed on the basis of radical trapping and electron spin resonance results. This finding illustrates a potential utilization of bimetallic MOF-derived metal phosphide as a photocatalyst to remove dye pollutants in the environment.
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高影响因子
CATALYSIS LETTERS
·
2015
·Vol. 145
·期 3
·784-793
·
IF 2.307
Zhang Xuejun,Zhang Peipei,Yu Hongbo,Ma Zhen,Zhou Shenghu
Abstract Bimetallic PdM (M = Ni, Co, Fe) nanoparticles were synthesized using butyllithium as a reductant, and were used to prepare Pd–M
x
O
y
/KIT-6 catalysts by appropriate oxidation and reduction treatments. These catalysts showed higher selectivity in the hydrogenation of p -chloronitrobenzene to p -chloroaniline than Pd/KIT-6. Relevant characterization was conducted using X-ray diffraction, transmission electron microscopy, N 2 adsorption–desorption, X-ray photoelectron spectroscopy, inductive coupled plasma emission spectrometer, and H 2 temperature-programmed reduction. Graphical Abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Fangxin Deng,Shoushu Wei,Xiangwei Zhang,Yanping Zhu,Qingze Chen,Zhiyi Deng,Runliang Zhu
A novel single-atom-like Co/Fe catalyst (i.e., Co/Fe-N-C) was synthesized by pyrolysis of a Zn/Co/Fe zeolitic imidazolate framework, and applied in peroxydisulfate (PDS) activation for removal of organic contaminants from wastewater. The isolated diatomic metal-nitrogen sites were detected by X-ray adsorption fine-structure. The degradation of four contaminants (i.e., phenol, bisphenol A, 2,4-dichlorophenol, and N-methyl-2-pyrrolidone) with a concentration of 100 mg/L could be degraded separately within 20 min by the Co/Fe-N-C system with 10 mmol/L of PDS, 0.5 g/L of catalyst dosage, and initial pH of 3. Besides, 79.2 % of phenol could be mineralized in 120 min, and the turn-over frequency value of the catalyst was calculated to be 27.17 min −1 , which was higher than the commonly reported homogeneous PS-AOPs. Moreover, the Co/Fe-N-C exhibited high stability (mineralization rate over 70 % after 5 cycles), a wide initial pH range (3−9), and high catalytic performance at 5–20 mmol/L of PDS concentrations. Based on the analysis of radical scavenging experiments and electron spin resonance spectra, the radical and non-radical pathways for PDS activation were proved in the system, and the contribution of phenol degradation by each pathway was clarified.
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ACS Catalysis
·
2024
·
IF 11.3
Ying Zhang,Junjun Mao,Bo Zhang,Dan Wang,Chenchen Zhang,Yang Lou,Chengsi Pan,Yongfa Zhu
Electrochemical carboxylation of 1,3-dienes with carbon dioxide (CO2) is a feasible method to obtain dicarboxylic derivatives, which are important synthetic intermediates of polymers and pharmaceuticals. However, due to unavoidable byproducts and unfriendly conditions, the formation of pure dicarboxylic acids has been limited. In this work, we report that a bimetallic phosphating CoFeP catalyst on nickel foam (CoFeP/NF) served as a remarkable electrode, which transforms CO2 into multicarbon (C6+) dicarboxylic acids. The synergistic effects of CoFeP catalyst between Co and Fe allow activation of 1,3-dienes mainly, in which electron transfer easier to the 1,3-dienes proceeded to afford radical anion of the diene, pursuant carboxylation with CO2 and further electron transfer formed the ultimate carboxylated products. The reaction can occur in a commercial flow cell with gram-scale amplification. The dicarboxylic acid obtained was up to 1.08 g at a 5 mmol scale of 1,3-dienes, illustrating high electrocatalytic activity and practical application of CoFeP/NF.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yunqing Pi,Lingjia Ma,Peng Zhao,Yangdan Cao,Huiqin Gao,Chunfeng Wang,Qilu Li,Shuying Dong,Jianhui Sun
A kind of Co-Fe Prussian blue analogues (Co-Fe PBAs), cobalt hexacyanoferrate Co 3 [Fe(CN) 6 ] 2 , and graphene oxide (GO) were combined to synthesize magnetically separable Co-Fe PBAs@rGO nanocomposites through a simple two-step hydrothermal method. The crystalline structure, morphology and textural properties of the Co-Fe PBAs@rGO nanocomposites were characterized. The catalytic performance of the nanocomposites was evaluated by PMS activation, with Levofloxacin Hydrochloride (LVF) as the target contaminant. Synergistic interactions between the Co-Fe PBAs and rGO prevented the aggregation of the Co-Fe PBAs nanoparticles, which resulted in enhanced degradation efficiencies. The influence of several critical parameters was investigated, including the reaction temperature, PMS and Co-Fe PBAs@rGO catalyst concentrations, solution pH and salt content. LVF degradation was favored at higher catalyst and PMS concentrations, high temperatures, and in neutral or weak acidic solutions. Sulphate radicals were the dominant active species in the Co-Fe PBAs@rGO/PMS system. In addition, the Co-Fe PBAs@rGO exhibited no significant decrease in LVF degradation efficiency following five catalytic cycles. Thus, the as-prepared Co-Fe PBAs@rGO nanocomposite catalyst might be applied to the removal of hard-to-degrade organics owing to its high catalytic ability to activate PMS, as well as its good reusability and recyclability.
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高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2025
·
IF 2.3
Chunlai Wu,Aimaiti Gali,Chuanyun Peng,Yalei Miao,Juan Li,Xinyu Gao
The treatment of dye wastewater is of crucial significance for alleviating water pollution, ensuring ecological security and achieving the sustainable utilization of water resources. In this work, the 1-allyl-3-butylimidazolium chloride ionic liquid modified Co/Fe-LDH (Co/Fe-LDH@IL) was successfully synthesized and explored for elimination Methylene Blue (MB) from aqueous solutions. Characterizations revealed that the incorporation of ionic liquids notably increased the specific surface area from 5.37 m2.g−1 to 8.15 m2.g−1. Additionally, the number of surface active sites, was significantly enhanced. For a 25 mL MB solution with an initial concentration of 300 mg.L−1, the optimal dosage of Co/Fe-LDH@IL was determined to be 30 mg, achieving adsorption equilibrium within 20 min. Under these conditions, the maximum adsorption capacity was 517.43 mg.g−1. Kinetic studies indicated that the pseudo-second-order model accurately described the process. The Langmuir isotherm model provided a better fit than the Freundlich model, indicating a homogeneous monolayer adsorption mechanism. Column adsorption experiments further validated the superior performance of Co/Fe-LDH@IL in treating MB solutions of different concentrations. The adsorption mechanism involved electrostatic interactions, interface regulation by IL molecules, and monolayer π-π interaction adsorption on imidazole functional group. Co/Fe-LDH@IL exhibits outstanding adsorption performance and stability, showing great potential for efficiently treating MB-containing wastewater.
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