CATALYSIS LETTERS
·
2026
·Vol. 156
·期 9
·261
·
IF 2.5
Su Qiqi,Dai Wanrong,Liu Meijun,Cheng Mengyu,Dai Chunyan,Li Yafei
The rational design of non-noble metal catalysts relies on a deep understanding of the structure-performance relationship. Herein, we investigate the influence of pyrolysis temperature (800–1100 °C) on Co–N/C catalysts derived from ZnCo-ZIF for the aerobic oxidation of 5‑hydroxymethylfurfural (HMF) to 2,5‑furandicarboxylic acid (FDCA). A volcano‑shaped dependence of FDCA yield on pyrolysis temperature is observed, with the catalyst pyrolyzed at 1000 °C (Co–N/C-1000) delivering complete HMF conversion and 98.0% FDCA yield within 4 h under optimized conditions (110 °C, 2 MPa O 2 ). Multi-technique characterization reveals a temperature-driven evolution of Co species: from atomically dispersed Co–N x sites at 800–900 °C, to a bimodal configuration comprising abundant Co–N x together with a small amount of metallic Co 0 nanoparticles at 1000 °C, and finally to large Co aggregates at 1100 °C. The optimal catalytic performance at 1000 °C is thus attributed to this unique coexistence. Kinetic analysis confirms the consecutive pathway HMF → HMFCA → FFCA → FDCA with FFCA→FDCA as the rate‑determining step. Notably, the optimal catalyst maintains 96.8% FDCA yield under industrially relevant 5 wt% HMF concentration. This work provides insights into the structure-performance relationship of Co–N/C catalysts and a rational strategy for designing efficient non-noble metal catalysts for biomass conversion. Graphical
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ACS Applied Materials & Interfaces
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2026
·
IF 7.8
Wenxuan Lu,Simin Wang,Yuxuan Xu,Xiaoxia Wang,Xijun Wang,Kun Zhao,Yunfei Gao,Fuchen Wang
The integration of an intermetallic Pt alloy and single-atom M–N–C support is an intriguing strategy to combine the advantages of both counterparts and further lower Pt usage at higher power output. Despite prior attempts, the fuel cell performance is still unsatisfactory, and the atomic diffusion/alloying pathway between the Pt alloy and M–N–C is still not clear. Here, we control the Co amount in the CoNC and present the atomic-diffusion pathway for the in situ formation of Pt-based intermetallic catalysts with size-controlled nanoparticles (NPs). The synthesized Pt3Fe–Co@5CoNC demonstrates excellent performance in half-cell ORR tests. Under H2–air conditions, the membrane electrode assembly exhibits low Pt usage (0.175 g kW–1), good stability with a 12.5 mV loss at 0.8 A cm–2 at the end of the test, and an ultrahigh power density of 1.717 W cm–2 at 0.429 V. Comprehensive experimental results and DFT calculations show the atomic pathway of diffusion and alloying for low-coordinated Co–N3–C into L12-Pt3Fe NPs. In comparison, high-coordinated Co–N4–C remains stable and contributes to the stability of the intermetallic Pt alloy through the strong Pt–Co–N4 interaction. This work demonstrates important progress in the integration of intermetallic Pt alloy and single-atom CoNC for ORR and can be extended to other single-atom supports, including Ni-NC, Fe-NC, and Cu-NC.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Dege Xili,Qian Zhou,Lijuan Zhang
Non-precious metal nitrogen-carbon composites (M-N-C) derived from ZIFs are an excellent non-precious metal catalyst for use in energy conversion and storage devices such as fuel cells and metal-air batteries. Herein ZIF-67 precursor with good dispersion, perfect crystal structure and size of below 270 nm was synthesized by consuming low amount of 2-methylimidazole ligand using a mixture of ethanol (EA) and methanol (MT) as the reaction medium. Compared with the traditional method of reducing the size of ZIF-67 by increasing the amount of ligands in methanol, this method avoids the waste of raw materials and saves the cost. The Co-N-C-MT/EA catalysts derived from ZIF-67 exhibits good ORR activity in alkaline media (0.1 M KOH) with a half-wave potential of 0.81 V vs RHE. After 5000 cycles, the initial potential and half-wave potential basically remain no change, showing excellent long-term stability. And remarkable methanol resistance is also displayed comparing with commercial Pt/C. The present experimental result shows that the improved synthesis method of ZIF-67 precursors has far-reaching implications for the field of catalyst research.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shiping Shao,Shuzhi Xing,Ke Bi,Tingting Zhao,Hao Wang,Yunxiang Tang,Jiurong Liu,Fenglong Wang
The fabrication of dielectric/magnetic multicomponent hybrids represents a promising strategy for achieving advanced electromagnetic wave (EMW) absorption performances. However, it also poses a significant challenge due to the difficulty in fully utilizing the properties of each component. Here, in this work, metal–organic frameworks (MOFs) derived Co-N-C species were combined with graphene oxide/polyamide acid and then freeze-dried and annealed to produce PI/rGO/CNC aerogels. These aerogels exhibit outstanding EMW absorption properties owing to their multiple heterogeneous interfaces and synergetic electromagnetic losses while retaining satisfying mechanical properties and lightweight features of PI/rGO aerogels. In particular, PI/rGO/CNC-1 aerogel shows the optimal EMW attenuation performance with a minimal reflection loss (RL min ) value of –75 dB, and its maximal effective absorption bandwidth (EAB max ) is as broad as 7.28 GHz. Moreover, the lightweight nature, elastic feature, structural stability, thermal insulation and hydrophobicity of the PI/rGO/CNC aerogels ensure that they have vast application prospects as advanced EMW absorption materials in complicated environment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Gongheng Zhang,Abdullah Ali Mohammed Ahmed Al-Anzah,Fengxiang Yin,Jie Zhang,Guoru Li,Biaohua Chen,Qiuyue Gao,Xian Tong Yu,Yuqian Sun
The precursor ZIF-67/xC-T was prepared by solvothermal and pyrolysis methods. A series of ZIF-67/xC-T-yIL catalysts were then prepared by modifying the surface of the precursor with [BMIM][NTf 2 ] ionic liquid . The results showed that [BMIM][NTf 2 ] as sulfur and nitrogen sources, N, S co-doped carbon can improve the catalytic activity of ORR . Meanwhile, [BMIM][NTf 2 ] formed an oxygen-rich layer on the catalyst surface, which increased the contact between oxygen and the active sites, reduced the alkaline strength of the catalyst surface, and improved the desorption ability of the catalyst to the product. Therefore, the ZIF-67/xC-T-yIL catalyst exhibited better ORR activity in an alkaline electrolyte than the catalyst without [BMIM][NTf 2 ]. Among the ZIF-67/xC-T-yIL catalysts, ZIF-67/1.2 C-600–6IL demonstrated the best ORR catalytic activity, with a half-wave potential of 0.86 V and a limiting current density of 5.21 mA cm −2 in 0.1 mol L −1 KOH, which was comparable to that of commercial 20% wt% Pt/C.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Huijie Wang,Hongzhao Chen,Qingqiao Wan,Yuzhao Zheng,Yang Wan,Xin Liu,Xianghai Song,Wei Ma,Pengwei Huo
In this work, a Co-N/C@CeO 2 composite material was successfully synthesized via hydrothermal, in-situ growth, calcination methods and applied in a thermal-assisted activation peroxymonosulfate (PMS) system for efficient degradation of polyethylene terephthalate microplastics (PET MPs). The effects of various parameters, including catalysts, reaction temperature, H 2 O 2 , PMS dosages and catalyst loading, on the degradation efficiency of PET MPs were systematically investigated. Characterization techniques, including mass spectral (MS) analysis, in-situ Fourier transform infrared (in-situ FT-IR) and electron paramagnetic resonance (ESR), revealed that PET MPs adsorbed on the surface were rapidly degraded under the action of hydroxyl radical (•OH) and sulfate radical (SO 4 •− ). In the presence of a small amount of H 2 O 2 and the synergistic effect, the Co-N/C@CeO 2 composite material successfully achieved a 92.3% degradation rate of PET MPs in the thermal-assisted activation PMS system. DFT calculations indicated that the Co-N/C@CeO 2 composite material exhibited relatively lower adsorption energy and higher activation capacity for HSO 5 − molecules. In addition, toxicity assessment results showed that the degradation intermediates had generally lower toxicity. This study not only provides valuable insights for the construction of high-activity Co-N/C and CeO 2 composite materials but offers technical and theoretical guidance for the effective degradation of PET MPs in the environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yi Gao,Xinyang Tan,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
The water treatment performance of membrane filtration is usually restricted via the paradox between permeability and selectivity. Herein, the nitrogen doped porous carbon supported Co catalysts (CoNPC), serving as both porous filler and peroxymonosulfate (PMS) activator, were firstly filled into polyvinylidene fluoride (PVDF) matrix to construct a novel mixed matrix catalytic membrane (CoNPC@PVDF) for enhanced water purification. Owing to the robust binding between CoNPC and PVDF, a high loading (50 wt%) and even dispersion of CoNPC were realized in CoNPC@PVDF, and its permeability and selectivity were both improved with the increase of CoNPC content. The optimum CoNPC@PVDF with PMS activation assistance (FCP) exhibited effective phenol removal at short retention time (1.5 s) and high permeability (256.6 L m −2 h −1 bar −1 ). The performance of CoNPC@PVDF FCP was 2.9 and 2.5 times higher than that of filtration alone and PMS activation alone, respectively, and even dramatically outweighed the reported catalytic membranes and heterogeneous catalysts. The outstanding performance of CoNPC@PVDF catalytic membrane was mainly attributed to its thin membrane structure and high filling degree of CoNPC, resulting in ultrahigh mass transfer rate (1.8 × 10 −4 m s −1 ) and more exposed active sites for enhanced PMS activation into radicals (mainly •OH and SO 4 •− ) towards pollutant removal.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Dan Wang,Peixia Yang,Hao Xu,Jingyuan Ma,Lei Du,GuoXu Zhang,Ruopeng Li,Zheng Jiang,Yun Li,Jinqiu Zhang,Maozhong An
The Zn-air battery is a promising next-generation battery because of the higher energy density and safety compared with the Li-ion battery. However, the Zn-air battery suffers from huge energy loss and poor cycling performance, which are due to the sluggish kinetics of oxygen reduction/evolution reactions (ORR/OER) and the instability of bifunctional catalysts . The state-of-the-art bifunctional catalyst is the composite of Pt and Ir/Ru oxides, which is hindered by the scarce resource and high cost. Therefore, developing low-cost and high-efficient bifunctional non-noble metal-based catalysts is essential to the deployment of Zn-air batteries. Herein, we report a dual-nitrogen-source mediated pyrolysis route to rationally design and synthesize the hybrid Co/Co–N–C bifunctional catalyst. The tailored catalyst consisting of carbon confined Co nanoparticles and atomically dispersed Co–N–C moiety is identified. Remarkably, the dual-nitrogen-source derived Co/Co–N–C catalyst demonstrates excellent electrochemical performances with a half-wave potential of 0.882 V for ORR and a potential of 1.640 V at 10 mA cm −2 for OER; reasonably, the bifunctionality of Co/Co–N–C, which is supported by the excellent self-breathing Zn-air battery performance (the maximum energy density of 897.1 Wh kg Zn −1 ; no obvious degradation within 167h cycling). The abundant Co-Nx sites and metallic Co nanoparticles synergistically boost the ORR and OER.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 21.1
Zhishuai Yuan,Jixiang Zou,Weijie Hong,Mei Yan,Chongshen Guo,Lei Zhao,Zhenbo Wang
The production of hydrogen peroxide via the two-electron oxygen reduction reaction has emerged as a sustainable route for electro-Fenton technology in wastewater treatment, yet it remains challenged by the competing four-electron pathway and the lack of atomic-level structure-selectivity relation explanation, especially in acidic media. Here, precisely engineered CoN 3 O 1 atom sites are constructed by substituting an N atom with an O atom in CoN 4 coordination, thereby realizing atomic-level regulation of the first coordination shell in Co-N-C catalyst. Density functional theory (DFT) calculations and advanced spectroscopy reveal that precise O substitution for N modulates the Co electronic structure and spin state, optimizes *OOH adsorption free energy, and inhibits O-O bond cleavage. As a result, CoN 3 O 1 delivers higher than 90% H 2 O 2 selectivity. In situ Raman and isotope-labeled differential electrochemical mass spectrometry (DEMS) capture the *OOH intermediate and further verify the 2e - pathway. In bio-electro-Fenton system, CoN 3 O 1 realizes 97.9% tetracycline removal and high mineralization efficiency without consuming external electrical energy. This work clarifies the role of atomic-level oxygen coordination engineering in governing 2e - ORR selectivity and provides a general design principle for advanced single-atom catalysts in bio-electro-Fenton systems.
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Environmental Science-Nano
·
2024
·Vol. 11
·期 5
·2010-2020
·
IF 5.8
Yanqing Cong,Lingjie Ye,Qiuang Zheng,Yudi Wang,Yifan Shao,Xuhua Ren,Shi-Wen Lv
Water pollution has always been an issue of significant human concern, and the development of effective wastewater treatment processes is important. Herein, three Co–N/C-based catalysts with different types of nitrogen were fabricated and employed to activate peroxymonosulfate (PMS) for tetracycline (TC) degradation. Due to the existence of a spatial confinement effect, all the Co–N/C-based catalysts showed excellent catalytic activities, and the removal efficiencies of TC were over 90% within 10 min. Notably, current results indicate that the Co–N/C-based catalyst rich in pyridinic N provides electrons to break the peroxy bonds of PMS for generating SO4˙−, while the Co–N/C-based catalyst containing more pyrrolic N acquires electrons from PMS to produce SO5˙−, which is further converted into 1O2. Moreover, the Co–N/C-based catalyst rich in graphitic N displayed good performance in electron transfer and can mediate the direct electron transfer process between TC and PMS. More interestingly, radical-induced oxidation exhibited a high TOC removal efficiency, but the corresponding anti-interference ability was weak. 1O2-induced oxidation and direct electron transfer process had a high removal efficiency for TC and good anti-interference ability, but the mineralization efficiency was relatively low. In short, the current work will provide a valuable reference for future research.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 27
·13050-13061
·
IF 9.931
Chaozhong Guo,Yanrong Li,Wenli Liao,Yao Liu,Zhongbin Li,Lingtao Sun,Changguo Chen,Jin Zhang,Yujun Si,Lu Li
The improvement of total nitrogen content and nitrogen-doping efficiency in carbon-based electrocatalysts is greatly significant to boost the electrocatalytic activity for the oxygen reduction reaction (ORR). Here, we report a new strategy for the synthesis of a highly mesoporous cobalt and nitrogen co-doped carbon electrocatalyst (3D-Co–N–C) with a three-dimensional network structure and a high BET surface area (∼638 m2 g−1) via using a novel cobalt-2,4,6-tri(2-pyridyl)-1,3,5-triazine complex with a strong molecular-level coordination effect as a single-source precursor and self-assembled sodium chloride aggregates as a space-confined nanoreactor for effective control of a high-temperature calcination process to reduce the thermal loss of nitrogen atoms and promote the nitrogen-doping efficiency, facilitating boosting of the ORR electrocatalytic activity in alkaline medium. The prepared 3D-Co–N–C catalyst exhibits unexpectedly excellent ORR activity with an onset potential of ∼1.0 V and a half-wave potential of ∼0.83 V, which is comparable to that of the commercial 20 wt% Pt/C catalyst. Additionally, the H2O2 yield (<17.0%) and the average electron transfer number of ∼3.8 for 3D-Co–N–C indicate a quasi four-electron pathway for ORR catalysis, suggesting that 3D-Co–N–C is a promising carbon-based electrocatalyst. It is proposed that the formation of the Co–Nx active structure can effectively enhance the electrocatalytic activity, but high contents of pyridinic- and graphitic-N can be mainly responsible for the ORR activity, which may be the electrocatalytically active site centers for the ORR. Besides, high BET surface area, highly mesoporous characteristics and outstanding electronic conductivity are also significant for the improvement of ORR activity. This study can provide a new, facile and green method for building high-performance carbon-based ORR electrocatalysts derived from easily available and innoxious transition metal–organic complexes, which can also help us to better understand the origin of the activity, active sites and their catalysis mechanism.
研究领域:
材料化学
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电催化
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纳米材料科学
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能源化学
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物理化学
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环境功能材料
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先进能源技术
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ChemSusChem
·
2019
·Vol. 12
·期 4
·830-838
·
IF 7.804
Shuai Wang,Haeseong Jang,Jia Wang,Zexing Wu,Xien Liu,Jaephil Cho
Graphical From tannic acid to water splitting : Amorphous Co−P/Co−N−C supported on N, P co-doped porous carbon (Co−P/Co−N−C/NPC) with a large specific surface area and abundant reactive sites is prepared. The material exhibits outstanding catalytic performance for the hydrogen evolution reaction (HER, η =234 mV at 10 mA cm −2 ), oxygen evolution reaction (OER, η =374 mV at 10 mA cm −2 ), and oxygen reduction reaction (ORR, E 1/2 =0.89 V, vs. RHE). It remains a tremendous challenge to develop a low-cost, earth-abundant, and efficient catalyst with multifunctional activities for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). Herein, a facile and scalable avenue was developed to prepare amorphous Co−P/Co−N−C supported on N, P co-doped porous carbon (Co−P/Co−N−C/NPC) with a large specific surface area (1462.9 m 2 g −1 ) and abundant reactive sites including Co−P, Co−N and NPC. The prepared electrocatalyst exhibits outstanding catalytic performance for HER ( η =234 mV at 10 mA cm −2 ), OER ( η =374 mV at 10 mA cm −2 ), and ORR ( E 1/2 =0.89 V, vs. reversible hydrogen electrode). Benefiting from the excellent HER performance and outstanding OER activity, the Co−P/Co−N−C/NPC delivers a current density of 10 mA cm −2 for overall water splitting at a cell voltage of 1.59 V, which is comparable with the IrO 2 –Pt/C couple electrode.
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