ACS Catalysis
·
2021
·
IF 13.084
Lipeng Wu,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Herein, a series of Co@N–C materials are synthesized using nitrates (LiNO3, NaNO3, and KNO3) as templates to control the preferential growth of the cobalt (200) facet. Co@N–C–X (X = LiNO3, NaNO3, and KNO3) exhibit excellent activities and long-term stabilities for Fenton-like degradation of bisphenol A (BPA) with peroxymonosulfate (PMS) as an oxidant. The texture coefficient (TC) is used to investigate the relationship between the Co facets and their catalytic activities, and a linear relation is built between the TC of Co(200) and the reaction rate constant (k). Co(200) is therefore the most active facet for PMS activation, while nitrates can promote the preferential growth of the Co(200) facet. Moreover, the Co(200) facet is more stable against leaching and can achieve more quick transformation between Co2+/Co3+. Quenching tests, electron paramagnetic resonance spectra, and electrochemical tests show that singlet oxygen (1O2) plays the dominant role for BPA degradation. Density functional theory verifies that Co nanoparticles coated with a graphitic nitrogen-doped carbon layer have the best activity for PMS activation. This work first proposes the strategy of using nitrates to control the preferential growth of Co facets and reveals the relationship between the TC value and k, thus attracting great interest in the environmental field.
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高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Haikuo Lei,Yanli Ruan
The slow kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) significantly limit the performance and broader applications of zinc-air batteries. To address this, a series of M-N-C catalysts were synthesized using W,O-doped ZIF-67 as a precursor. By modifying the surface electronic structure through doping and improving oxygen intermediate adsorption, these catalysts demonstrated excellent bifunctional catalytic activities for OER and ORR. Among them, W,O-CoNC700 achieved the half-wave potential and overpotential of 0.81 V and 359 mV, respectively. DFT calculations revealed that doping with W atoms affected the d-band center of the Co site, thus enhancing its catalytic ability. The maximum power density of a W,O-CoNC700-based zinc-air battery reached 174.8 mW/cm², outperforming the commercial Pt/C + IrO₂ catalysts. Under constant current discharge at 5 and 10 mA/cm², the cell maintained 1100 and 450 h, respectively.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Jiaming Cui,Xiaoting Cao,Xi Wang,Jie Liu,Ningyi Yuan,Jianning Ding
The strategic development of high-efficiency electrocatalysts for the oxygen reduction reaction (ORR) remains a pivotal challenge in advancing high-performance zinc-air batteries (ZABs) towards commercial viability. In this work, we developed a template-directed synthesis of Co, N-co-doped polyhedral carbon 3D frameworks (Co-N-C-x) through controlled pyrolysis of Co-ZIF precursors grown on Co-ZnO nanorod self-template. Owing to its unique carbon skeleton architecture and uniform dispersion of Co and N species, the optimized catalyst (Co-N-C-7%) exhibits enhanced ion/electron-transfer kinetics, improved mass transport capabilities. Consequently, the Co-N-C-7% catalyst exhibits superior ORR performance, achieving a half-wave potential (E1/2 = 0.878 V vs. RHE) that is 3 mV higher than commercial 20 wt% Pt/C (E1/2 = 0.875 V vs. RHE), along with exceptional stability. When applied in ZABs, the Co-N-C-7% cathode delivers a higher peak power density (178 mW cm-2) compared to Pt/C-based counterparts (152 mW cm-2). This work provides a simple and reliable control scheme for designing cost-effective, high-performance, and durable ORR electrocatalysts.
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ENERGY & FUELS
·
2025
·
IF 5.3
Yingrui Wang,Guanzheng Yang,Ming Chao,Jiaqing Zhao,Wen-tao Wang,Jin Yan,Qunying Wang,Ruizhi Yang
The oxygen reduction reaction (ORR) is a critical reaction in many renewable energy conversion and storage systems, such as fuel cells and metal-air batteries. High price, poor stability, and scarcity of Pt-based electrocatalysts, which are commonly used for ORR, limit the development of fuel cells and metal-air batteries. Transition-metal and nitrogen codoped carbons (M–N–C) are deemed as promising alternative electrocatalysts for ORR. Nevertheless, achieving sufficient ORR activity with M–N–C still faces great challenges. Here, cobalt (Co)-decorated Co–N–C coupled with MXene (Co/Co–N–C@MS-MXene) catalysts are successfully prepared via an in-situ construction of ZIF-derived Co–N–C at the surface of MXene etched by a Lewis acid molten salt. The as-synthesized Co/Co–N–C@MS-MXene delivers a superior ORR catalytic activity with a half-wave potential of 0.75 V vs RHE and a diffusion-limiting current density of 5.1 mA cm–2. A 4-electron transferring process and high stability are enabled. The excellent ORR performance can be attributed to the highly active Co-decorated Co–N–C and strong electronic coupling of Ti–O–Co between Co–N–C and MS-MXene, which promote the catalytic kinetics of ORR. This work demonstrates a universal, efficient, and green approach for the in-situ construction of active sites on MXene substrates.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xiaoju Li,Saijun He,Guangdong Yang,Jing Ma,Li Yuan,Xingbin Yang,Zhong Zhang
The excessive use of nitrite (NO 2 − ) has become a major food safety concern, posing a significant threat to public health. Therefore, developing a rapid, accurate, and on-site detection method for NO 2 − is of practical importance. Unlike peroxidase-mimicking nanozymes, oxidase-mimicking nanozymes can directly utilize molecular O₂ as an oxidant to produce ROS, eliminating the requirement for exogenous oxidants such as H₂O₂. Here, cobalt nitrogen doped carbon nanozymes (Co–N/C) with enhanced oxidase-like activity were synthesized by spatial confinement pyrolysis of ZIF-67. The hollow architecture of Co–N/C enhanced both the specific surface area and the density of active sites, thereby boosting oxidase-like catalytic performance. Substrate screening and theoretical calculations revealed that TMB exhibited the LUMO energy level (−0.0222 eV), lower than those of other tested substrates. Leveraging the diazotization reaction of NO 2 − , a paper-based visual detection platform was constructed, and enabling on-site quantification of NO 2 − . The method showed high selectivity, with a detection limit of 0.31 μM, well below national safety standards. This system was successfully applied to the determination of sodium nitrite in sausage, creating a promising strategy for the development of integrated, intelligent point-of-care testing systems.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Jiang Li,Jiaxing Liu,Junjie Zhang,Tong Wan,Lei Huang,Xintian Wang,Runze Pan,Zhidong An,Dionisios G. Vlachos
Cobalt (Co) catalysis has recently attracted significant attention in the field of biomass conversion. However, the fabrication of highly dispersive Co nanoparticles at high metal loading with selective facet exposure to achieve specific selectivity is still questionable. In this work, a nitrogen-doped carbon-supported Co catalyst is fabricated for efficient conversion of fatty acids and esters to liquid alkanes. Nitrogen-doping facilitates a highly uniform dispersion of Co nanoparticles even at a high Co loading of 10 wt% and after recycling for 5 runs. The Co/N-C catalyst affords an unconventional decarbonylation/decarboxylation (DCOx) dominant selectivity probably due to partial reduction of cobalt oxides to α-Co 0 with only exposure of the (111) facet. Co-existence of Co and N-C leads to strong Lewis acidity and basicity, facilitating the interaction between catalyst and –COOH group, and some important acid-catalyzed step-reactions. The versatility of the Co/N-C catalyst is demonstrated through conversion of various fatty acids and esters.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Minghuan Wang,Hekai Zhang,Yunfei Song,Yilei Zhu,Yaning Zong,Peng Wei,Zheng Guo,Li Yin,Jianwei Fu
s The practical application of metal-organic framework (MOF)-derived catalysts in advanced oxidation processes (AOPs) is often hindered by challenges in recoverability and stability in complex water matrices. To overcome these limitations, we developed a scalable strategy to fabricate N-doped carbon nanofibers with coexisting atomic Co sites and metallic Co nanoparticles (Co-N/C) by electrospinning a ZIF-67/polyacrylonitrile (PAN) composite followed by controlled pyrolysis. This integrated design yields a catalyst with a hierarchical porous structure and a high specific surface area (317.55 m 2 g -1 ), which synergistically enhances mass transfer and exposes abundant active sites. The optimized Co-N/C catalyst demonstrates ultrafast catalytic activity, achieving over 98% degradation of methylene blue (MB) within 5 minutes via efficient peroxymonosulfate (PMS) activation. Mechanistic studies, supported by quenching experiments and density functional theory (DFT) calculations, reveal that the degradation proceeds via a nonradical-dominated pathway, with singlet oxygen ( 1 O 2 ) generated through interfacial electron transfer playing the primary role, while sulfate (SO 4 • - ) and hydroxyl (•OH) radicals from Co 2+ /Co 3+ redox cycling serve a secondary function. The catalyst exhibits excellent operational robustness, maintaining high efficiency (>92%) across a broad pH range (3-9) and showing remarkable reusability with minimal activity loss over five consecutive cycles. Furthermore, ecological structure-activity relationship (ECOSAR) modeling indicates a significant reduction in the environmental toxicity of the degradation intermediates. This work provides not only an effective and eco-friendly candidate for dye wastewater remediation but also fundamental insights into the rational design of MOF-derived functional materials for superior, nonradical-predominant AOPs.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
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IF 5.2
Ke Wu,Chunlei Wu,Wenou Bai,Ning Li,Yangqin Gao,Lei Ge
Hydrogen energy is vital important for solving pollution of environment and energy shortage. Hydrogen production via solar energy and semiconductor photo-splitting water is one of the most environmentally friendly strategies at present. In this work, Co-N-C, a non-noble metal-based ZIF-67 derivative, was employed as a co-catalyst to achieve an in situ growth of spherical CdS via simple one-step hydrothermal. Due to the large specific surface area of Co-N-C, the agglomeration of CdS is avoided and the photocorrosion phenomenon is weakened. Under irradiation of visible light , the hydrogen generation activity of Co-N-C/CdS was achieved 905 μmol g −1 h −1 . It is 6 times that of pure CdS with excellent stability. At the contact interface of the Co-N-C and CdS, the transfer and the separation of photoinduced carriers had been enhanced by a great many of channels. DFT calculation further showed that Co nanoclusters , as the active sites of hydrogen production, significantly enhanced photocatalytic hydrogen evolution activity. Therefore, Co-N-C not only acts as electron acceptor , but also serves as support of highly dispersed CdS to promote the stability of system during photocatalytic hydrogen generation. This work demonstrates the advantages of CdS binding MOF derivatives to construct composite photocatalysts with enhanced dispersibility and hydrogen production activity.
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Reaction Kinetics Mechanisms and Catalysis
·
2020
·Vol. 129
·期 2
·865-881
·
IF 1.52
Liu Minjie,Zhang Hao,Wang Junyan,Zhao Guoming,Liu Di
A Co–N–C catalyst was fabricated via pyrolysis–reduction process. Dehydrogenation/hydrogenation and base catalysis performances of the Co–N–C catalyst were investigated by using the reductive coupling of nitroarenes with alcohols and aldol condensation as probe reactions. Various characterizations were performed to explore effects of reduction and pyrolysis temperature on the structure/composition and basicity of the Co–N–C catalyst, and the relationship between structure-dehydrogenation/hydrogenation and base catalysis performance was discussed accordingly. Two different structures of Co–N–C catalyst (Co–N–C/C 3 N 4 and Co–N–C/CNT) were obtained in different pyrolysis temperature. Co–N–C-600 with C 3 N 4 exhibits very weak catalytic performance owe to its poor pore system and active phase. Dehydrogenation/hydrogenation behaviors of Co–N–C/CNT depend on the amount of Co–N, graphitic N in Co–N–C, while the basicity of Co–N–C is closely related to the content of N species, particularly pyrrolic N and pyridinic N. The appropriate pyrolysis temperature benefits the formation of active species, developed pore organization and strong basicity. And, the H 2 reduction improve dehydrogenation/hydrogenation activity of Co–N–C/CNT because reduction can destroy carbon coating layers to expose more Co–N species and promote the transformation of N species to graphitic N. Meanwhile, H 2 reduction increases the contents of graphitic N and reduces the content of pyrrolic N and pyridinic N, thus weakening catalyst basicity and consequently reducing base catalytic activity of Co–N–C/CNT.
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ACS Catalysis
·
2024
·
IF 11.3
Zhengyu Zhao,Zongxuan Yang,Hongmei Bai,Hongwei Zhang,Bowen Zhang,Xinru Wu,Zimeng Li,Cejun Hu,Xiaojun Bao,Pei Yuan
Aqueous-phase hydrogenation holds significance in achieving the large-scale green production of succinic acid, but the acidic reaction environment poses a considerable challenge in the design of highly active and stable catalysts. Herein, we report a spatial-confinement strategy to fabricate a CoNPs@Co-N-C core–shell structured catalyst where Co nanoparticles (CoNPs) are encapsulated tightly by nitrogen-doped graphitic carbon shells (NG), while Co single atoms (CoSA) are distributed homogeneously on the shells, which exhibits remarkable efficiency and stability in the aqueous-phase hydrogenation of maleic acid for the production of succinic acid in an acidic medium. The catalyst achieves 100% conversion of maleic acid, more than 98% selectivity toward succinic acid, and high stability for seven cycles without significant deactivation. The combined characterizations and density functional theory (DFT) calculations further indicate that CoNP and CoSA can concurrently optimize the electronic structure of the NG and promote hydrogen dissociation on the surface of the carbon shells. These findings shed light on the unique function of CoNP-NG-CoSA composite sites on regulating the hydrogenation active centers and provide a guideline for the further development of highly efficient acid-resistant hydrogenation catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Zehao Tan,Guiru Zhang,Jun Li,Enping Wang,Liuxuan Luo,Shuiyun Shen,Junliang Zhang
Single-atom catalysts (SACs) have received extensive attention due to their theoretically 100 % atomic utilization, low cost and unique catalytic performance. In this work, CoNi@CoNCs were prepared via impregnation-reduction method. CoNi@CoNCs possess coexisting Co–N–C SAC and CoNC-coated CoNi dilute alloy nanoparticles (NPs), in which Co NPs are doped with trace Ni amount. After optimizing the Co/Ni atomic ratio and heat treatment temperature, the CoNi@CoNCs exhibit exceptional acidic oxygen reduction reaction (ORR) activity with a half-wave potential of 0.754 V and a double-layer capacitance of 48.42 mF cm −2 in 0.1 M HClO 4 solutions. After 10,000 cycles of degradation test, the half-wave potential of the Co 8 Ni 1 @CoNC-600(Co 8 Ni 1 Co/Ni atomic ratio 8:1 in the precursor; 600 = heat treatment temperature 600 °C) only decreased by 35 mV. According to advanced and comprehensive experimental and theoretical analyses, the reasons for the improvement toward acidic ORR activity and stability of the CoNi@CoNC can be attributed to the following several reasons.(1) the Co 2+ and Co–N electron structures influenced by the trace Ni amount.(2) The unique CoNC-coated structure. (3) The synergistic effect between CoNi NPs and Co single atoms. This work helps to expound the specific role of NPs in SACs, providing theoretical guidance for the further development of non-noble metal NPs and single-atom co-component catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Kun Geng,Pengnian Shan,Lijing Wang,Feng Guo,Weilong Shi
Carbon-based materials have attracted considerable attention in the field of photothermal catalysis owing to their exceptional chemical stability, wide-range light harvesting and high photothermal conversion efficiency. In this work, ZIF-67 was pyrolyzed at different temperatures to produce Co-N-C materials with varying graphitization degrees, revealing that lower graphitization leads to superior photothermal performance. Herein, they are employed as heat-core material and integrated with ZnIn 2 S 4 (ZIS) to form composites via a water-bath method for photothermally promoted photocatalytic H 2 production. Experimental resutls reveals that the low-graphitized Co-N-C features abundant structural defects to construct highly active surface sites and exhibits a strong localized surface plasmon resonance (LSPR) effect that efficiently converts photons into phonons, thereby elevating the local surface temperature of the catalyst. Meanwhile, the interfacial interaction formed between the low-graphitized Co-N-C and ZIS in Co-N-C@ZIS composite effectively promotes the separation and migration of photogenerated electron-hole pairs, thereby enhancing the performance of the photothermal-assisted photocatalytic H 2 generation with achieving an H 2 generation rate of 14.09 mmol g −1 h −1 under full-spectrum illumination, 12.04-fold higher than pure ZIS (1.17 mmol g −1 h −1 ). The work provides valuable insights and strategies for significantly enhancing photothermally promoted photocatalytic hydrogen evolution through the utilization of carbon-based heat-core materials.
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