Journal of CO2 Utilization
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2019
·
IF 5.189
Weiqi Liu,Zhichao Miao,Zhenbin Li,Xiaozhong Wu,Pengfei Zhou,Jinping Zhao,Huahua Zhao,Weijiang Si,Jin Zhou,Shuping Zhuo
A series of Co@N-C materials are synthesized from pyrolysis of ZIF-67 at different temperatures and employed as catalyst for electrochemical reduction of CO 2 (CO 2 RR) to syngas. Through a systematical investigation of the relationship between structure of Co@N-C catalysts and their catalytic activity, it could be found that the Co species exposed on the material surface mainly promote the hydrogen evolution reaction (HER) process to produce H 2 , while the Co particles packaged by N-C skeleton provide electrons and transfer them to CO 2 molecule through the Co -N- C skeleton, promoting the CO 2 reduction reaction. Following this thinking, the pristine Co@N-C materials are treated by aqua regia to remove the surface exposed Co species. After acid treatment, the affinity of H species sharply decreases, and adsorption of CO 2 and transfer of electron to CO 2 are successfully improved. The acid-treated Co@N-C catalysts exhibit improved catalytic activity, faradic efficiency of CO, and stability in CO 2 RR process. Among all these catalysts, the obtained Co@N-C-700-A shows highest CO 2 reduction activity and stability, achieving a specific current of 25 A∙g (cat) −1 and a productivity of 0.266 mol (CO) h −1 ∙ g(cat) −1 at a mild potential of -0.57 V vs. RHE. The ratio of CO/H 2 in products could be adjusted in the range of 1/4 to 1.5/1.
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NEW JOURNAL OF CHEMISTRY
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2026
·
IF 2.6
Zefan Liu,Xuejiao Rong,Jianchao Ma,Yin Xiao,Lin Shuo Jiang,Yang Li,Xilong Yan,Ligong Chen,Bowei Wang
The development of M-N-C catalysts (M = Fe, Co, Ni, etc.) was hindered by poor distribution of metal species and large particle size. In this work, alkaline additives were introduced during the precursor synthesis stage to regulate the distribution of metal components. Through hydrothermal and pyrolysis methods, Co-N-C catalysts (Co-N-C-NH3, Co-N-CO3, and Co-N-C-OH) were synthesized by using folic acid as the carbon and nitrogen source, cobalt chloride as metal salt, and ammonia solution, sodium carbonate solution, and sodium hydroxide solution as alkaline additives, respectively. The influence of different alkaline additives on the morphology, composition, and structure of Co-N-C catalysts was systematically analyzed through systematic characterization methods. The results indicated that the Co-N-CO3 catalyst prepared using sodium carbonate solution has a largest specific surface area, smallest and most evenly distributed Co nanoparticles. Moreover, the catalytic activity of the prepared Co-N-C catalyst in the hydrogenation of nitrobenzene was evaluated, and the influence of alkaline additives on its catalytic performance was further explored. Among them, the Co-N-CO3 catalyst achieved the best in the hydrogenation of nitrobenzene after reacting at 110 °C and under 1 MPa hydrogen for 3 hours, with a nitrobenzene conversion rate of over 99%. Comparative experiments confirmed that Co nanoparticles and Co-Nx sites constituted the active centers of the catalytic reaction. This strategy provides theoretical support and practical basis for optimizing the performance of Co-N-C catalyst.
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JOURNAL OF MATERIALS RESEARCH
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2026
·
IF 2.9
Zhang Zhiwei,Nie Yuhang,Zhang Lianke,Wei Zhiqiang,Li Dandan,Qin Haiying,Ni Hualiang,Li Yangyang,He Junjing
Atomically dispersed catalysts, characterized by their high atom utilization efficiency and distinct catalytic activity, exhibit advantages in reducing fuel cell costs. Herein, we synthesized Co/N/C atomic catalysts by acid leaching of CoO/N/C prepared through carbothermal shock. The resulting Co/N/C-130 demonstrates outstanding performance for the oxygen reduction reaction (ORR) in alkaline media. It displays a half-wave potential ( E 1/2 ) of 0.82 V and a Tafel slope of 47.1 mV dec −1 . Furthermore, it exhibits excellent stability with a positive E 1/2 shift of 6 mV after 40,000 cycles. When applied as a cathode catalyst in a direct borohydride fuel cell (DBFC), Co/N/C-130 achieves a maximum power density of 396 mW cm −2 at 60 °C. Long-term durability test at 50 mA cm −2 reveals a power retention of 90.8% after 24 h and 76.3% after 50 h. These results demonstrate that Co/N/C-130 atomic catalyst is a highly efficient and durable non-precious metal catalyst for ORR. Graphical abstract
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 6
·981-987
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IF 3.1
Nan Li,Minghao Shi,Wei Zhan,Wenjing Shen,Mianmian Wu,Guifang Sun,Qingfei Li,Jiangquan Ma
Ru-based catalysts are potential substitutes for Pt in the hydrogen evolution reaction (HER). It is worth noting that the Se ions in RuSe2 can modulate the electronic structure of the Ru metal, thus effectively improving the HER kinetics of RuSe2. However, single electronic structure modulation is hard to complete due to the electron deficiency of active Ru atoms. Herein, we prepare and design a novel RuSe2/Co–N–C (RuSe2 nanospheres supported on Co–N–C nanosheets) electrocatalyst with two-electron modulation by a hydrothermal and thermal annealing method. Benefiting from the uniform distribution of RuSe2 nanospheres on Co–N–C nanosheets and Co–N–C nanosheets acting as additional electron donors to make up for the electron deficiency of the Ru metal, RuSe2/Co–N–C exhibits excellent HER performance with a low overpotential of 26.4 mV at 10 mA cm−2 and a low Tafel slope of 53.2 mV dec−1. This work offers an effective method for the synthesis of high catalytic performance electrocatalysts by constructing an interaction between the carrier and the active metal.
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NANO
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2026
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IF 1.3
Keqiang Zhu,Jincheng Wang,Xinxin Tan,Zhiyong Jia,Yun Wang,Chuang Zhang
Developing efficient and cost-effective oxygen reduction reaction (ORR) catalysts is crucial for advancing clean energy technologies. In this study, the 3D polypyrrole aerogel was synthesized using methyl orange as a soft template. The subsequent in-situ spatially confined pyrolysis ensures the atomic dispersion of Co-N x active sites while effectively suppressing metal agglomeration. The optimized CoNC-150 catalyst exhibited a high surface area (298.53 m 2 /g) and well-distributed cobalt-coordinated active sites (Co-N 4 ), significantly enhancing ORR performance. Electrochemical evaluations demonstrated an exceptional half-wave potential of 0.886 V, closely approaching that of commercial 20 wt% Pt/C (0.892 V). The catalyst followed a fourelectron transfer pathway, ensuring efficient ORR kinetics. Remarkably, this robust 3D monolithic architecture endows the catalyst with exceptional stability in alkaline media. Long-term durability tests over 40,000 cycles confirmed their remarkable stability, with only a 0.008 V loss in half-wave potential, significantly lower than the 0.022 V loss in Pt/C under similar conditions. The degraded CoNC-150 exhibited a half-wave potential of 0.878 V, significantly outperforming Pt/C (0.870 V). Kinetically, CoNC-150 exhibits a Tafel slope of 146.16 mV/dec, indicating favorable ORR dynamics. These results highlight the potential of CoNC-150 as a highly active and durable non-precious metal catalyst (NPMC) for ORR applications. This study provides valuable insights into the rational design of transition metal-based electrocatalysts, offering a promising route toward scalable and sustainable energy conversion technologies.
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RSC Advances
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2026
·Vol. 16
·期 14
·12524-12536
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IF 6.1
Zhaopeng Sun,Yaling Wu,Yingying Chen,Zhibo Li,Sen Lei,Yongyong Cao,Lianwen Zhu,Xuebo Cao,Zheng Yan
Previous studies have often focused on optimizing electrocatalytic performance by altering the type of metal centers or the morphological structure of catalysts to modulate their electronic structures and active sites. However, the precise regulation of metal valence states to enhance catalytic performance—particularly for trifunctional electrocatalysis in the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER)—remains in the exploratory stage. In this study, crystalline Co–N6 materials with controllable valence states were carefully selected as precursors. Through carbonization, Co–N–C materials with similar carbon frameworks but distinct metal valence states (Co2+ and Co3+) were successfully prepared. Both experimental tests and theoretical calculations demonstrate the superior trifunctional electrocatalytic performance of Co2+–N–C. Density functional theory (DFT) calculations provide evidence for the more favorable intermediate adsorption energies and lower reaction energy barriers exhibited by Co2+–N–C. This performance advantage stems from the 3d7 electronic configuration of Co2+, which optimizes electron cloud density and strengthens Co–N bonding interactions. This work presents a new strategy for designing highly efficient electrocatalysts by elucidating the regulatory role of metal valence states.
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高影响因子
Advanced Composites and Hybrid Materials
·
2021
·Vol. 4
·期 4
·1292-1301
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IF 5.693
Zhang Pengxiang,Zhang Xihua,Li Bin,Xu Lingan,Dang Feng,Li Bao-Wen
Improving the interfacial impedance matching and attenuation ability of a microwave absorber is an important strategy to obtain excellent microwave absorbing performance. Here, we prepared an ultralight, hierarchical porous single-atom Co–N–C microwave absorber, in which evenly distributed single-atom Co is anchored in a porous N-doped carbon framework by N–Co bond via a facile bio-inspired method. These doped single atoms provide abundant highly active atomic absorption sites on the carbon skeleton, and considerable defects including pyridinic-N, pyrrolic-N, oxidized N, and so forth are introduced into the carbon framework owing to single Co atom doping. These doped single Co atoms and introduced defects act together as strong dipolar/interfacial polarization units, which lead to better impedance matching and a significant increase in attenuation capability of the absorber. The metal Co exists in form of a single atom, benefiting light weight of the absorber. Therefore, an extremely strong reflection loss (RL) value of − 60.9 dB is achieved at a lower filler content of 10 wt% with the absorber thickness of 2.5 mm, and the effective frequency bandwidth covered from 10.4 to 15.1 GHz with a thickness of 2.0 mm at a low filler content of 10 wt%. This research offers a novel route for designing a microwave absorber to improve microwave absorption performance and is expected to a wider range of absorbing materials with different structures. Graphical abstract
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ACS Catalysis
·
2021
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IF 13.084
Muhong Li,Shanyong Chen,Qike Jiang,Qingliang Chen,Xuan Wang,Yong Yan,Jian Liu,Changchang Lv,Weiping Ding,Xuefeng Guo
The production of functionalized anilines by chemoselective hydrogenation of nitroarenes occupies an important position in the chemical industries. Recently, cobalt and nitrogen codoped carbon (Co–N–C) catalysts have been reported to show outstanding catalytic performance in this process, whereas the nature of their active sites is still at the center of intense debate. In this paper, based on the well-controlled experiments on four types of typical Co–N–C materials derived from different methodologies, several unusual generalities in the hydrogenation of nitroarenes are clearly revealed, including protic-solvent dependence, antipoisoning, acid resistance, and reversible deactivation. Further investigations indicate that the single-atom species Co–Nx are the main active sites of the Co–N–C catalysts in this chemoselective hydrogenation process. The present work sheds light on the mechanism study on the metal–N–C catalysts and further contributes to the rational design of the high-performance single-atom catalysts.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Zhiyan He,Guangxing Yang,Hongjuan Wang,Fengying Dai,Feng Peng,Hao Yu
Metal- and nitrogen-doped carbon materials (Me–N–C) have received intensive scientific interest as single-atom catalysts (SACs) for electro- and thermocatalytic reactions. In this work, the potential of Me–N–C (Me = Co, Fe, Ni)-wrapped carbon nanotubes (CNTs) as support of platinum nanoparticles (Pt NPs) for base-free oxidation of glycerol was investigated. Co-doping of transition metal and nitrogen significantly enhanced the dispersion of Pt, indicating the advantages of the supporting material for noble-metal catalysts. Two-fold improvement of turnover of glycerol was observed over 5Pt/CoNC@CNT compared to 5Pt/CNT under the same reaction conditions. A kinetics study was conducted to understand the role of CoNC as a support of Pt NPs in a wide range of oxygen partial pressure from 0.04 to 0.4 MPa and a range of glycerol concentration from 0.012 to 0.15 wt %. A synergistic effect between Me–N–C, especially Co–N–C, and Pt NPs was revealed. The Co–N–C support facilitated the activation of oxygen and thus enhanced the overall turnover of glycerol oxidation, especially at high glycerol concentrations. This finding suggests a new approach to the high-performance Pt catalysts via introducing SACs as supporting materials that afford auxiliary active sites for the target reaction.
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CHEMOSPHERE
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2024
·
IF 8.1
Mu Li
The release of organic dyes, such as Rhodamine B (RhB), into industrial wastewater has led to significant issues with color pollution in aquatic environments. Herein, we prepared a cobalt nanoparticles (NPs)-based catalyst with the nitrogen-doped carbon-support (Co@N–C) for effective PMS activation. The Co@N–C/PMS system demonstrated the excellent catalytic activity of Co@N–C for activating PMS, achieving nearly 100% degradation of RhB. Singlet oxygen ( 1 O 2 ) and sulfate radicals (SO 4 • - ) were dominant reactive oxygen species for RhB degradation. Density functional theory (DFT) calculations substantiated that the production of 1 O 2 commenced with the initial generation of *OH through hydrogen abstraction from PMS, culminating in the direct release of oxygen to form 1 O 2 (PMS→*OH→O*→ 1 O 2 ). The generation of SO 4 • - was attributed to electron transfer to PMS from the surface of Co NPs (Co 0 →Co 2+ →Co 3+ ) and the C–N shell (Co 2+ →Co 3+ ). The research findings provided new insights into the development of Co-based heterogeneous catalysis for advanced oxidation of refractory organic pollutants in wastewater treatment.
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Nanoscale
·
2024
·Vol. 16
·期 10
·5215-5221
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IF 5.8
Yangdong Zhou,Junda Chen,Zhiyin Huang,Yuqin Peng,Lixin Xing,Chunmei Tang,Ning Wang,Ling Meng,Mingjie Wu,Lei Du,Siyu Ye
The cathodic oxygen reduction reaction (ORR) has been continuously attracting worldwide interest due to the increasing popularity of proton exchange membrane (PEM) fuel cells. So far, various Pt-group metal (PGM) or PGM-free catalysts have been developed to facilitate the ORR. However, there is still a gap to achieve the expected goals as proposed by the U.S. Department of Energy (DoE). Recently, PGM-free@PGM hybrid catalysts, such as the M/N/C@PtM catalyst, have achieved the milestones of oxygen reduction, as reviewed in our recent work. It is, nevertheless, still challenging to unravel the underlying structure–property relationships. Here, by applying different Pt/Co ratios, a series of Co/N/C@PtxCo catalysts are synthesized. Interestingly, the ORR activity and stability are not linear with the Pt content, but show a volcano-like curve with increased Pt usage. This relationship has been deeply unraveled to be closely related to the contents of pyrrolic N, pyridinic N, and graphitized carbon in catalysts. This work provides guidelines to rationally design the coupled PGM-free@PGM catalysts toward the ORR by appropriate surface engineering.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 8
·2129-2137
·
IF 9.405
Di Liu,Ping Yang,Hao Zhang,Minjie Liu,Wenfei Zhang,Dongmei Xu,Jun Gao
A non-noble heterogeneous catalyst – a Co, N and C composite encapsulated carbon nanotube grown in situ on the surface of activated carbon (Co–N–C/CNT@AC) – was fabricated via the pyrolysis–reduction process. Co–N–C/CNT@AC catalyzed the reductive coupling of structurally diverse nitroarenes and alcohols to imines and secondary amines under exogenous base- and solvent-free conditions. BET, TEM, SEM, XRD and XPS characterization showed that the exceptional catalytic property of Co–N–C/CNT@AC could be explained by its nanostructure, Co–N and basic N species. Our protocol had advantages of low cost, environment-friendliness, and good applicability. Furthermore, a reaction route of nitroarenes, amines and alcohols as the starting materials was proposed to improve the atom economy of the reductive coupling of nitroarenes with alcohols.
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