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学者姓名：谢在来
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Abstract ：
Borocarbonitride (BCN) catalysts, boasting multiple redox sites, have shown considerable potential in alkane oxidative dehydrogenation (ODH) to olefin molecules. However, their catalytic efficiency still lags behind that of leading commercial catalysts, primarily due to the limited reactivity of oxygen functional groups. In this study, a groundbreaking hybrid catalyst is developed, featuring BCN nanotubes (BCNNTs) encapsulated with manganese (Mn) clusters, crafted through a meticulous supramolecular self-assembly and postcalcination strategy. This novel catalyst demonstrates a remarkable enhancement in activity, achieving 30% conversion and approximate to 100% selectivity toward styrene in ethylbenzene ODH reactions. Notably, its performance surpasses both pure BCNNTs and those hosting Mn nanoparticles. Structural and kinetic analyses unveil a robust interaction between BCNNTs and the Mn component, substantially boosting the catalytic activity of BCNNTs. Furthermore, density functional theory (DFT) calculations elucidate that BCNNTs encapsulated with Mn clusters not only stabilize key intermediates (& horbar;B & horbar;O & horbar;O & horbar;B & horbar;) but also enhance the nucleophilicity of active sites through electron transfer from the Mn cluster to the BCNNTs. This electron transfer mechanism effectively lowers the energy barrier for & horbar;C & horbar;H cleavage, resulting in a 13% improvement in catalytic activity compared to pure BCNNTs. Manganese (Mn) cluster promoters enhance the catalytic activity of borocarbonitride in ethylbenzene oxidative dehydrogenation with approximate to 100% styrene selectivity, superior to these of unmodified and Mn particle-modified borocarbonitride materials, and the nature of activity improvement and reaction mechanism is revealed by combining with structural characterizations and density functional theory calculations. image
Keyword ：
borocarbonitride nanotubes borocarbonitride nanotubes heterogeneous catalysis heterogeneous catalysis Mn modfication Mn modfication oxidative dehydrogenation oxidative dehydrogenation strong interaction strong interaction
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| GB/T 7714 | Zhang, Xuefei , Dai, Xueya , Xie, Zailai et al. Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube [J]. | SMALL , 2024 , 20 (37) . |
| MLA | Zhang, Xuefei et al. "Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube" . | SMALL 20 . 37 (2024) . |
| APA | Zhang, Xuefei , Dai, Xueya , Xie, Zailai , Qi, Wei . Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube . | SMALL , 2024 , 20 (37) . |
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Carbon materials have stimulated tremendous interest in oxidative dehydrogenation (ODH) of alkane to olefin molecules at low temperature. Unfortunately, its further development has been seriously hindered due to the unsatisfactory catalytic performance. To tackle these challenges, nitrogen and phosphorus codoped hollow carbon prisms (NPC) are designed with controllable surface functional groups through supramolecular preassembly and substitution reaction from guanine and hexachlorotriphosphazene. The resultant catalysts can achieve both high catalytic activity (63 % conversion) and styrene selectivity (90 %) in ODH of ethylbenzene, outerperforming previous reported carbon-based catalysts. Structural characterizations, kinetics measurements and theoretical results unravel that nitrogen doping can promote nucleophilicity of -C--O, thus improving the catalytic activity. The phosphorus doping not only changes reaction rate-determining step from activation of O2 in N-doped carbon to activation of -C-H bond of EB in N,P-codoped carbon, but also inhibits the formation of electrophilic oxygen species, which enhances selectivity of styrene. The current work provides a facile strategy for preparation of functional NPC catalyst and physical-chemical insights on the structure-activity relationship of NPC catalysts, paving the way for further development of the highly efficient non-metallic catalytic systems.
Keyword ：
Carbon prism Carbon prism Catalytic mechanism Catalytic mechanism Guanine Guanine Heteroatom doping Heteroatom doping Oxidative dehydrogenation Oxidative dehydrogenation
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| GB/T 7714 | Zhang, Xuefei , Hu, Aoxue , Li, Shuchun et al. N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
| MLA | Zhang, Xuefei et al. "N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity" . | CHEMICAL ENGINEERING JOURNAL 486 (2024) . |
| APA | Zhang, Xuefei , Hu, Aoxue , Li, Shuchun , Feng, Ruiping , Huang, Shuping , Xie, Zailai . N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity . | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
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The development of highly efficient bifunctional electrocatalysts with excellent stability at high current densities for overall water splitting is a challenging but urgent goal. Herein, a novel kind of significantly efficient bifunctional electrocatalysts has been elaborately designed through the fabrication of Fe-doped Ni2P nanosheets decorated with CeO2 nanoparticles (Fe-Ni2P/CeO2) grown on Ni foam. It reveals the existence of electron transfer from Ni2+ to Ce4+, resulting in an increase of Ni3+, of which the strong Lewis acidity promotes the adsorption of OH- and thus facilitates the formation and conversion of oxygen-related intermediates during the water splitting process. The resulting catalyst shows outstanding electrocatalytic activities for both oxygen evolution reaction (OER) (r20 = 190 mV, r1000 = 260 mV) and hydrogen evolution reaction (HER) (r20 = 78 mV, r1000 = 292 mV). Moreover, when utilized for overall water splitting, the Fe-Ni2P/CeO2 requires very low voltages of 1.52 V and 2.88 V to achieve current densities of 20 mA cm-2 and 1000 mA cm-2, respectively, outperforming the Pt/C || RuO2 electrolyzer. Importantly, the as-designed electrolyzer exhibits exceptional durability at a high current density of 1000 mA cm-2. This work has demonstrated an effective strategy for designing non-precious metal heterojunctions with abundant electrocatalytic active sites to drive efficient overall water splitting.
Keyword ：
CeO2 nanoparticles CeO2 nanoparticles Fe-dopedNi2P Fe-dopedNi2P Heterojunction Heterojunction High current densities High current densities Overall water splitting Overall water splitting
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| GB/T 7714 | Huang, Yuxin , Ding, Xueda , Huang, Baobing et al. CeO2-decorated Fe-doped Ni2P nanosheets for efficient electrocatalytic overall water splitting at high current densities [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 981 . |
| MLA | Huang, Yuxin et al. "CeO2-decorated Fe-doped Ni2P nanosheets for efficient electrocatalytic overall water splitting at high current densities" . | JOURNAL OF ALLOYS AND COMPOUNDS 981 (2024) . |
| APA | Huang, Yuxin , Ding, Xueda , Huang, Baobing , Xie, Zailai . CeO2-decorated Fe-doped Ni2P nanosheets for efficient electrocatalytic overall water splitting at high current densities . | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 981 . |
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Iron-nitrogen-carbon (Fe-N-C) catalyst has emerged as highly promising contender for oxygen reduction reaction (ORR), yet challenges such as limited active site accessibility and intricate synthesis procedures impede their commercialization as a replacement for the benchmark Pt/C catalyst. Herein, we present an innovative approach to in situ fabricate a unique iron and nitrogen co-doped 3D porous carbon material. The material is synthesized through a straightforward one-step pyrolysis of xanthine, oxidized carbon nanotubes and iron nitrate nonahydrate mixture. During the high temperature pyrolysis, the nucleobase xanthine undergoes gradually transformation into an efficient N-doped graphene-like material. Simultaneously, it assembles with carbon nanotubes (CNTs), resulting in the formation of a unique 3D graphene-CNTs composite structure composed of graphene and CNTs. This exceptional 3D porous structure serves as an excellent scaffold, ensuring firm anchoring, uniform dispersion, and optimal exposure of numerous FeNx active sites. Leveraging this well-engineered framework, the optimized Fe-N-C catalyst (NC/CNT/Fe0.04) shows excellent ORR performance with an onset potential of 1.03 V vs. RHE, a half-wave potential of 0.87 V vs. RHE, and a diffusion-limited current density of −5.59 mA cm−2, even better than those of the commercial Pt/C catalyst. This work provides valuable insights into the design of efficient electrocatalysts with 3D channel. © 2024 Elsevier Ltd
Keyword ：
Carbon nanotubes Carbon nanotubes Catalyst activity Catalyst activity Doping (additives) Doping (additives) Electrocatalysts Electrocatalysts Electrolytic reduction Electrolytic reduction Graphene Graphene Iron compounds Iron compounds Nitrogen Nitrogen Oxygen Oxygen Porous materials Porous materials Pyrolysis Pyrolysis Scaffolds Scaffolds
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| GB/T 7714 | Huang, Baobing , Liu, Qianyi , Li, Yaxiang et al. Xanthine-derived 3D porous iron–nitrogen-carbon catalysts for enhanced oxygen reduction reaction [J]. | Fuel , 2024 , 371 . |
| MLA | Huang, Baobing et al. "Xanthine-derived 3D porous iron–nitrogen-carbon catalysts for enhanced oxygen reduction reaction" . | Fuel 371 (2024) . |
| APA | Huang, Baobing , Liu, Qianyi , Li, Yaxiang , Peng, Yixin , Xie, Zailai . Xanthine-derived 3D porous iron–nitrogen-carbon catalysts for enhanced oxygen reduction reaction . | Fuel , 2024 , 371 . |
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Iron and nitrogen co-doped carbon-based catalysts have garnered significant attention for their efficacy in the degradation of Rhodamine B (RhB), Tetracycline (TC) and other organic pollutants through peroxymonosulfate (PMS) activation. However, designing catalysts with both high activity and abundant active sites has proven challenging, primarily due to the limited understanding of the structure-activity relationship. Herein, we present a straightforward synthesis of iron and nitrogen co-doped carbon nanosheets (FeNC) that exhibit exceptional activity in activating PMS for degradation of RhB and TC. The FeNC material shows robust resistance to interference across a wide pH of 1.5 to 10, resistance to inorganic anions and humic acid (HA). More importantly, the Fe3C nanoparticles are uniformly anchored within the carbon layer, effectively prevent metal leaching. Unlike the traditional sulfate radical-based advanced oxidation processes, our study reveals that non -radical singlet oxygen (1O2) serves as the main reactive oxygen species (ROS) responsible for the degradation processes through quenching tests and electron paramagnetic resonance (EPR) analysis. Structural characterizations and spectroscopic study indicate that the potential active sites on FeNC, namely C--O, graphitic and pyridinic nitrogen play an important role in this degradation. Particularly noteworthy is the discovery that Fe3C species, present in the FeNC-900/PMS system, also contribute significantly to the degradation of TC. Moreover, we have proposed potential degradation pathways for RhB and TC based on the results of liquid chromatograph mass spectrometer (LC -MS) measurement. Overall, this study offers novel insights into the development of heterogeneous iron and nitrogen co-doped carbon-based catalysts for advanced oxidation processes (AOPs) via PMS activation.
Keyword ：
Degradation Degradation Guanine Guanine Iron and nitrogen co-doped Iron and nitrogen co-doped Rhodamine B Rhodamine B Tetracycline Tetracycline
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| GB/T 7714 | Li, Shuchun , Ke, Yiling , Zhang, Xuefei et al. Iron carbide nanoparticles encapsulated in guanine-derived carbon for peroxymonosulfate activation [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 338 . |
| MLA | Li, Shuchun et al. "Iron carbide nanoparticles encapsulated in guanine-derived carbon for peroxymonosulfate activation" . | SEPARATION AND PURIFICATION TECHNOLOGY 338 (2024) . |
| APA | Li, Shuchun , Ke, Yiling , Zhang, Xuefei , Wu, Shuchang , Xie, Zailai . Iron carbide nanoparticles encapsulated in guanine-derived carbon for peroxymonosulfate activation . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 338 . |
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5-Hydroxymethylfurfural (HMF) is a widely used biomass platform chemical that plays a crucial role in bridging biomass and fossil resources. Electrocatalytic oxidation of HMF provides an efficient way to obtain high-value-added biomass-derived chemicals, among which the intermediate product 5-formyl-2-furan carboxylic acid (FFCA) has attracted considerable attention. However, the weak adsorption ability of monometallic nickel oxide (NiOx) to HMF in neutral electrolyte restricts its further development, resulting in low HMF conversion and FFCA yield. In this study, we successfully constructed a novel nickel oxide-platinum oxide hybrid catalyst supported on carbon felt (NiOx-PtOx/CF), which exhibits an optimized adsorption ability of HMF, leading to the outstanding FFCA yield up to 77 % in the neutral media. The high activity of the NiOx-PtOx/CF catalyst can be attributed to the redistribution of the electrons and the optimization of the electronic structure on the Ni active site due to the introduction of PtOx on NiOx nanosheets. This study offers valuable insights for the design of efficient multicomponent electrocatalysts for electrocatalytic biomass refinery systems. Highly efficient of HMF into FFCA on a NiOx-PtOx/carbon felt composite electrode is achieved at a potential of 1.78 VRHE with high value product of FFCA yield up to 77 %. The high activity of the NiOx-PtOx/CF catalyst can be attributed to the redistribution of the electrons and the optimization of the electronic structure on the Ni active site due to the introduction of PtOx on NiOx nanosheets. image
Keyword ：
5-hydroxymethylfurfural 5-hydroxymethylfurfural bimetallic catalysts bimetallic catalysts electronic regulation electronic regulation Electrooxidation Electrooxidation formyl-2-furancarboxylic acid formyl-2-furancarboxylic acid
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| GB/T 7714 | Wang, Di , Lu, Xingyu , Xu, Haiyan et al. Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts [J]. | CHEMCATCHEM , 2024 , 16 (18) . |
| MLA | Wang, Di et al. "Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts" . | CHEMCATCHEM 16 . 18 (2024) . |
| APA | Wang, Di , Lu, Xingyu , Xu, Haiyan , Dou, Jing , Zhang, Xuefei , Xie, Zailai et al. Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts . | CHEMCATCHEM , 2024 , 16 (18) . |
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Maximization the synergistic effect of each component in transition metal-carbon complexes is expected to improve the bifunctional oxygen electrocatalysis for rechargeable Zn-air batteries but is still challenging. Herein, nucleobase guanine is employed as a supramolecular precursor to generate the core (FeCo alloy)-shell (carbon) structure embedded in ultrathin graphene-like nitrogen-doped carbon nanosheets (FeCo@NCNSs) via a confinement pyrolysis strategy. Thanks to the generated core-shell structure and bimetallic synergistic effect, the as-prepared FeCo@NCNSs exhibits excellent electrochemical performance in both oxygen reduction reaction and oxygen evolution reaction. As a result, when served as the bifunctional air electrode for a practical Zn-air battery, FeCo@NCNSs exhibits a higher open-circuit voltage (1.553 V) and peak power density (197.30 mW cm-2), as well as the greatly improved long-term cyclic stability compared to the noble metal benchmarks. This work provides a promising approach to integrate various active sites for bifunctional oxygen electrocatalysis and inspires the exploration of simple but efficient electrocatalysts for energy storage and conversion.
Keyword ：
Bifunctional oxygen electrocatalysis Bifunctional oxygen electrocatalysis Core-shell structure Core-shell structure FeCo alloy FeCo alloy Guanine Guanine Rechargeable Zn-air batteries Rechargeable Zn-air batteries
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| GB/T 7714 | Lin, Xin , Cui, Longji , Ding, Xueda et al. Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 998 . |
| MLA | Lin, Xin et al. "Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries" . | JOURNAL OF ALLOYS AND COMPOUNDS 998 (2024) . |
| APA | Lin, Xin , Cui, Longji , Ding, Xueda , Chen, Yiquan , Wei, Qiaohua , Huang, Baobing et al. Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries . | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 998 . |
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Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of -0.55 to -0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at -0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm(-2) is achieved in a flow cell at -0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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| GB/T 7714 | Peng, Ying , Chen, Shuo , Hu, Zhengli et al. Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction [J]. | DALTON TRANSACTIONS , 2024 , 53 (23) : 9724-9731 . |
| MLA | Peng, Ying et al. "Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction" . | DALTON TRANSACTIONS 53 . 23 (2024) : 9724-9731 . |
| APA | Peng, Ying , Chen, Shuo , Hu, Zhengli , Yin, Mengqi , Pei, Lishun , Wei, Qiaohua et al. Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction . | DALTON TRANSACTIONS , 2024 , 53 (23) , 9724-9731 . |
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Boroncarbonitrides (BCNs) are recently developed new catalytic system for efficient oxidative dehydrogenation (ODH) of alkanes to alkenes. Herein, a series of novel hierarchical BCN materials are synthesized using asymmetric hydrogen bonds self -assembly between methylguanidine and boric acid, along with ammonia deposition. The XRD, S(T)EM, and XPS characterizations confirm the presence of ternary BCN solid solution covered by small serrated -like BCN nanosheets materials in the 2D plates. The unique hierarchical structure and developed mesoporosity of the BCN material contribute to its outstanding catalytic performance. The optimal catalyst delivers robust catalytic performance and long-term stability in the ODH of propane reaction with propylene and total olefin selectivity of 74.7% and 89.7% at a stable 20.4% propane conversion, much better than BCN sheets and h-BN catalyst. Results show that the in -situ formation of suitable amounts of amorphous BOX species within the BCN structure, along with the maintenance of the 2D skeleton at elevated temperatures, is a significant contribution in the enhanced ODH reactivity. Moreover, density functional theory calculation also demonstrates that the presence appropriate carbon content in BCN catalysts can significantly promote the ODH of propane reaction.
Keyword ：
BCN catalysts BCN catalysts Hierarchical nanosheets Hierarchical nanosheets Oxidative dehydrogenation of propane Oxidative dehydrogenation of propane
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| GB/T 7714 | Wang, Guangming , Hu, Aoxue , Duan, Qiwei et al. Hierarchical boroncarbonitride nanosheets as metal-free catalysts for enhanced oxidative dehydrogenation of propane [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 288 . |
| MLA | Wang, Guangming et al. "Hierarchical boroncarbonitride nanosheets as metal-free catalysts for enhanced oxidative dehydrogenation of propane" . | CHEMICAL ENGINEERING SCIENCE 288 (2024) . |
| APA | Wang, Guangming , Hu, Aoxue , Duan, Qiwei , Cui, Longji , Chen, Ziyi , Huang, Zelong et al. Hierarchical boroncarbonitride nanosheets as metal-free catalysts for enhanced oxidative dehydrogenation of propane . | CHEMICAL ENGINEERING SCIENCE , 2024 , 288 . |
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Tetracycline (TC) plays an essential role in both medical treatment and animal husbandry, but its abuse and accumulation in aquatic environments undoubtedly threatens ecosystems and human health. The advanced oxidation processes (AOPs) based on the activation of peroxymonosulfate (PMS) for the degradation of TC and other organic contaminants has attracted increasing attentions. Although metal-organic framework (MOF) derived transition metal-nitrogen-carbon material (MNC) shows fascinating potential for PMS activation, the direct carbonization of MOF makes limited active sites available for reaction due to serious agglomeration of the metal species together with the low yield of MNC catalyst. Herein, MOF composite (ZIF-67/NG) is designed via the in-situ growth of ZIF-67 on the N-doped graphene-like carbon (NG). The obtained Co@NC/NG after pyrolysis of ZIF-67/NG enabled the exposure of more active sites without notable aggregation of the Co nanoparticles. Co@NC/NG could effectively degrade TC via the activation of PMS and showed relatively good stability. Meanwhile, it was also highly active in wide pH range and the coexistence of inorganic anions as well as humic acid. Compared to bare ZIF-67 derived Co@NC, Co@NC/NG exhibited higher TOF value. The quenching ex-periments combined with EPR analysis indicated that both radical and non-radical routes were involved during the TC removal. Superoxide radicals, singlet oxygen and the surface bounded reactive oxygen species were important to the reaction. In comparison, sulfate radicals only made slight contribution and the effect of hydroxyl radicals could be omitted.
Keyword ：
Degradation Degradation MOF composite MOF composite Peroxymonosulfate Peroxymonosulfate Radical/non-radical pathway Radical/non-radical pathway Tetracycline Tetracycline
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| GB/T 7714 | Wu, Shuchang , Zhao, Min , Xia, Zhijun et al. Highly dispersed Co on N-doped carbon derived from metal-organic framework composite for enhanced peroxymonosulfate activation toward tetracycline degradation [J]. | DIAMOND AND RELATED MATERIALS , 2023 , 140 . |
| MLA | Wu, Shuchang et al. "Highly dispersed Co on N-doped carbon derived from metal-organic framework composite for enhanced peroxymonosulfate activation toward tetracycline degradation" . | DIAMOND AND RELATED MATERIALS 140 (2023) . |
| APA | Wu, Shuchang , Zhao, Min , Xia, Zhijun , Liu, Junhui , Chen, Yiquan , Lv, Xiangxing et al. Highly dispersed Co on N-doped carbon derived from metal-organic framework composite for enhanced peroxymonosulfate activation toward tetracycline degradation . | DIAMOND AND RELATED MATERIALS , 2023 , 140 . |
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