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.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhen Qiu,Guanda Shen,Zefeng Ruan,Xin Zeng,Hailu Fu,Yongfu Li,Bing Yu
The removal of organic pollutants in complex aqueous environments is often hindered by the presence of natural organic matter (NOM), such as humic acid (HA), which can interfere with pollutant degradation processes. Peroxymonosulfate (PMS) activation has emerged as a promising strategy for pollutant degradation; however, its efficiency is typically compromised by NOM interference. To address this challenge, this study develops a metal–organic framework (MOF)-derived Co-N@C hollow multi-shell nanoreactor (HoMS) that effectively isolates NOMs while targeting organic pollutants. The Co-N@C HoMS, synthesized via a “hierarchical temperature control, one-step pyrolysis” strategy, demonstrated superior catalytic performance in selectively degrading carbamazepine (CBZ) in the presence of HA. Over 99% of CBZ was removed within 10 min, even with HA present. Mechanistic studies revealed that PMS activation by Co-N@C HoMS for CBZ degradation involves both radical oxidation and electron transfer pathways. The unique size-exclusion effect of the Co-N@C HoMS selectively allows small molecules (CBZ) to pass through while blocking larger ones (HA), enabling rapid and selective pollutant degradation in complex environments. This work provides a novel solution for the efficient and selective removal of multi-component pollutants in complex environmental systems.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 18
·13143-13155
·
IF 2.993
Li Jie,Chen Chao,Qin Furong,Jiang Yongjia,An Hao,Fang Jing,Zhang Kai,Lai Yanqing
Cobalt–nitrogen-doped mesoporous carbon (Co–N–C) is synthesized as a host for lithium–sulfur batteries. With the Co–N–C composite as a sulfur host, the initial capacity of lithium–sulfur batteries is as high as 1290.8 mA h g −1 at 0.2 C, and Li–S batteries still exhibit good cycling stability and high capacity with a retained capacity of 795.7 mA h g −1 and a nearly 100% coulombic efficiency after 300 cycles. The good performance of Li–S batteries can be attributed to a higher specific surface area and pore volume of the carbon matrix and good chemical affinity of Co and N elements toward polysulfides. It is found that Co–N–C composite can effectively adsorb lithium polysulfide by physical, chemical adsorption and well inhibit the shuttle effect. In addition, Co–N–C composite which act as a catalyst can also significantly promote the conversion of polysulfide, accelerate the kinetics, thereby improving the performance of Li–S batteries.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiaoe Dang,Sining Yun,Yongwei Zhang,Jingjing Yang,Zhuolei Liu,Changwei Dang,Yinhao Wang,Yingying Deng
With the increasing energy demands and impending climate change, significant concerns have been raised over the metal–organic frameworks (MOFs)-derived porous carbons and their utilization for hydrogen evolution reaction (HER) and triiodide reduction reaction (IRR). However, the provision of high intrinsic activity, active-site accessibility, and structural stability of MOF-derived Co-embedded N-doped carbon (Co/N-C) for HER and IRR is challenging. In this work, core-shell MOF-in-MOF precursors are designed to construct novel double-shell N-C-in-Co/N-C electrocatalysts with nanorod- and rhombic dodecahedron-shaped hollow morphologies (NR-H-C and RD-H-C). The double-shell structured NR-H-C and RD-H-C significantly enhance the HER and IRR activity of Co-MOF-derived Co/N-C. Specifically, NR-H-C achieves a high N-content (10.35 at.%), large specific surface area (590.87 m 2 g −1 ), and hierarchical porous configuration (micropores and mesopores). When NR-H-C is applied as the HER catalyst in alkaline electrolyte, it exhibits an admired overpotential of 123 mV at 10 mA cm −2 and a Tafel slope of 51 mV dec −1 . The solar cell adopting NR-H-C as counter electrode for IRR achieves a high short circuit current density of 16.77 mA cm −2 , an open-circuit voltage of 0.745 V, a fill factor of 0.682, and a power conversion efficiency of 8.51%, higher than that of Pt-based solar cell (16.26 mA cm −2 , 0.744 V, 0.602, and 7.28%). The elucidatory Volmer-Heyrovsky HER mechanism and reversed Volmer-Heyrovsky IRR mechanism give a better understanding of the enhanced dual-functional activity of NR-H-C. This work provides an essential information for the rational design of high-performance dual-functional HER and IRR catalysts and further open up a new avenue for the construction of multicomponent MOFs in the energy conversion field.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
EES Catalysis
·
2025
·
IF 8.1
Jie Yang,Lifang Chen,Xuya Zhu,Wenwen Shi,Mengxue Huang,Chang Liu,Ruimin Ding,Lin Gan,Xi Yin
H2O2 -related electrochemical reactions, including two-electron oxygen reduction reaction (2e-ORR), H2O2 oxidation reaction (HPOR), and H2O2 reduction reaction (HPRR), have received significant attention for the electrosynthesis H2O2 and energy storage. Understanding the complex structure-activity relationships among 2e-ORR/ HPOR/HPRR and their connections is crucial for further developing highly efficient catalysts and working systems. Herein, we unveil these intricacies by employing model Co-N-C catalysts with well-defined active site configuration (Co-N4-pyrrolic and Co-N4- pyridinic ) in a combined experimental and computational approach. We report the higher 2e-ORR/HPOR but lower HPRR activity of CoN4-pyrrolic site than the CoN4-pyridinic site based on their reaction free energy landscapes remodeled considering the chemisorption steps of O2 and H2O2 . The results reveal that the binding free energy of *OOH (ΔG*OOH ) can only be utilized as a reliable descriptor for 2e-ORR/HPOR activity, but not indicative of HPRR activity, regardless of the scaling relationship of the common reaction intermediates ( *OOH or *OH). The HPRR activity of CoN 4 sites strongly depends on the H2O2 adsorption strength and configuration. These findings provide valuable insights into the design of catalysts for H2O2 -related electrochemical energy conversion and storage systems.
研究领域:
电化学
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催化
·
材料科学
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能量转换与存储
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2018
·
IF 0
Shanshan Jie,Congqiang Yang,Yuan Chen,Zhigang Liu
The highly dispersed active sites are desirable to optimize the atom efficiency. In this study, a series of novel cobalt grafted in N-doped carbon (Co-N-C) catalysts for selective oxidation of ethylbenzene are synthesized by heating a solution of cobalt porphyrin and peptides in ionic liquids, which are also characterized by techniques such as FT-IR, XRD, SEM-EDX, HR-TEM, and XPS. The results show that the as-prepared catalysts have an attractive catalytic performance, namely, 40% of ethylbenzene conversion and 75% of selectivity to acetophenone. Especially, the activity and selectivity of the as-prepared catalysts remain almost similar even after the 10th run. Moreover, the modified-complexometry method is verified to improve the dispersion of metal active sites. The remarkable catalytic performance of the as-prepared catalysts is attributed to the highly dispersed active sites and strong interactions between Co and N species in Co-N x moieties.
研究领域:
催化
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材料科学
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化学工程
·
分析化学
✓ 已验证
产品关联
DOI
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Jialu Wei,Jingyu Wang,Wei Zhang,Yuezhen Mao,Chunwen Sun
Graphical A ZAB with Co–N–C–PBMCRO cathodic catalyst achieves a remarkable cycling stability for 788 h. The perovskite Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) composite was constructed by in situ exsolved CoRu nanoparticles and Co–N–C with more exposing active sites. A conductive pathway for oxygen ions and electrons was built, thereby enhancing the electrochemical bifunctional properties. This rational design strategy shows great potential for facilitating synthesis of perovskite based catalysts for energy conversion and storage applications. Bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential components of rechargeable zinc-air batteries. In this study, we synthesized a Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) perovskite composite with in situ exsolved CoRu nanoparticles and Co–N–C, functioning as an efficient bifunctional electrocatalyst for zinc-air batteries. The in situ exsolution of CoRu nanoparticles from the perovskite oxide was facilitated by the reducing action of 2-methylimidazole (2-MIM). Concurrently, Co–N–C was used to decorate PBMCRO, forming a novel bifunctional composite electrode of Co–N–C–PBMCRO. The incorporation of CoRu nanoparticles introduces a significant number of electrochemically active oxygen vacancies in the perovskite matrix, enhancing ORR and OER performance. Additionally, the Co–N–C synergistically improves electrochemical activity while preserving the structural stability of the perovskite oxide. The prepared Co–N–C–PBMCRO catalyst demonstrates significantly enhanced bifunctional performance compared to the undecorated pristine perovskite Pr 0.5 Ba 0.5 MnO 3−δ (PBMO). The zinc-air battery with Co–N–C–PBMCRO catalyst achieve a peak power density of approximately 90 mW/cm 2 and exhibit remarkable cycling stability for 788 h. This study presents a novel and effective strategy to enhance the catalytic performance of perovskite-based air electrodes for rechargeable metal-air batteries.
研究领域:
材料科学
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电化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
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.
研究领域:
材料科学
·
电化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Miao Liu,Zhenghao Lu,Linghan Yang,Renmin Gao,Xinying Zhang,Yongjing Wang,Yonghao Wang
Electrocatalytic reduction of nitrate to ammonia is an effective method for the recycling of NO 3 - -N in the field of nitrate polluted water treatment . In this work, Co-N-C was prepared in this work by pyrolysis of Co-based metal organic framework at 700 °C and it can achieve 100 % selectivity to ammonia under the optimum experiment conditions. Impressively, no harmful nitrite generated in the reduction process because the reduction rate constant of Co-N-C for NO 2 - -N is higher than that of NO 3 - -N. Experiment results show that the chemical adsorption rather than electrostatic adsorption dominated among Co-N-C and free NO 3 - , which is significant for the subsequent electronic reduction process. Mechanism analysis indicated the active hydrogen (H*) reduction mechanism is predominate for Co-N-C but the direct electron mechanism is predominate for Co-C during the reduction from NO 3 - to NO 2 - . While for Co-N-C and Co-C, the subsequent reduction of NO 2 - to NH 4 + was conducted by the direct electron mechanism. The present work not only explores high performance for the selectively electrocatalytic reduction from nitrate to ammonia but also promote new inspiration for the preparation of other Co-based functional materials for reducing the production of nitrite.
研究领域:
环境科学
·
电催化材料
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 15
·7153-7160
·
IF 3.925
Weifeng Huang,Junqiang Li,Xiao Xu,Aihui Cao,Ying He,Miao Sun,Longtian Kang
Electrocatalytic reduction of CO2 with non-precious materials containing the Co–N–C moiety as a catalyst is considered to be a promising method to achieve carbon neutrality. Unfortunately, metal phthalocyanines with an intrinsic Co–pyrrolic N4–C structure usually show low electrocatalytic activity due to serious aggregation and low conductivity. Here, we exhibit a simple strategy to controllably disperse cobalt phthalocyanine (CoPc) on graphene oxide (GO) by the hydrolysis of protonated CoPc in GO aqueous phase. CoPc/GO nanocomposites with different ratios and structures could be easily obtained, and their effect on the electrocatalytic activity for the CO2 reduction reaction (CO2RR) to CO was systematically investigated. In the optimal sample, a CO selectivity of >96% can be achieved with an overpotential of <190 mV. Meanwhile, a CO Faradaic efficiency (FECO) of >90% can be reached within a wide potential range from −0.7 to −1.0 V (vs. RHE). The systematical experiments reveal that the synergy of CoPc and GO should be crucial owing to the existence of strong electrostatic interactions at the initial stage of hydrolysis and subsequent π–π, hydrogen bond and axial coordination interactions between CoPc and GO. This work exhibits a simple strategy to prepare molecule-based nanostructures as highly efficient electrocatalysts.
研究领域:
材料科学
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环境科学
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电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhuoran Ren,Fang Chen,Qin Zhao,Guoqiang Zhao,Hui Li,Wenping Sun,Hongwei Huang,Tianyi Ma
Piezocatalysis has attracted the increasing interest of researchers as a novel catalytic method. To date, there are two popular mechanisms regarding the piezocatalysis, i.e., the piezoelectric effect and the energy band theory. However, both mechanisms cannot fully explain the piezocatalytic process: the electrons generated by the piezoelectric effect will not spontaneously participate in the piezocatalysis, while not all piezoelectric materials have an appropriate energy band structure. In this work, displacement current and the principle of piezoelectric nanogenerator are introduced to fully comprehend the piezocatalytic mechanism for the first time. As a proof-of-concept catalytic system, we synthesize Co-N-C@BaTiO 3 piezocatalyst for the CO 2 reduction reaction (CO 2 RR) under ultrasonic vibration. A promising piezocatalytic CO 2 reduction rate of 261.8 mol g −1 h −1 is achieved with a high CO selectivity up to 93.8% under 50 kHz ultrasonic vibration. The CO yields of this catalytic system outperform most of the reported photocatalytic CO 2 RR and piezocatalytic CO 2 RR. Moreover, a comprehensive piezocatalytic mechanism from displacement current to active sites is proposed and supported by combining Co-N-C@BaTiO 3 piezoelectric nanogenerator, COMSOL simulation and energy band structure analysis. Under the ultrasonic vibration, the electrons generated by the piezoelectric effect are driven by the time-varying electrostatic potential formed by the displacement current. The suitable band structure of piezoelectric provider that satisfies the potential of reaction promotes electrons to participate in CO 2 RR on active sites. Overall, our work provides an insightful understanding of piezocatalysis and paves a new path for its development.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）