Reaction Chemistry & Engineering
·
2020
·Vol. 6
·期 1
·112-118
·
IF 3.441
Renjie Huang,Yanxin Wang,XiXi Liu,Peng Zhou,Shiwei Jin,Zehui Zhang
The selective hydrogenation of nitro compounds into their corresponding azo compounds is challenging in organic synthesis. In this study, we have developed a facile and efficient catalytic system for the transformation of nitro compounds into azo compounds under mild conditions over a heterogeneous cobalt catalyst (Co–Nx/C-800-AT). The Co–Nx/C-800-AT catalyst was found to be highly active for the reductive-coupling of nitro compounds into azo compounds in ethanol at 110 °C and 2.5 bar H2 pressure with the addition of NaOH as an additive, affording structurally-diverse azo compounds with satisfactory yields (70.4–98.3%). The developed method demonstrated several advantages such as high catalytic activity and high selectivity with tolerance to other functional groups and high stability.
研究领域:
有机化学
·
催化材料科学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wenfei Dong,Guo Chen,Mengyao Ding,Haiyan Cao,Gaoya Li,Meiqing Fang,Wenbing Shi
Nanozyme-based sensing strategy for glucose generally involves a two-step H 2 O 2 -bridged cascade reaction . However, this two-step cascade reaction always shows a limited detection efficiency for glucose, which hardly makes simply operation, rapid detection, and sensitivity all promised. Herein, a novel strategy for one-step glucose detection was proposed based on the efficiently competitive relationship between glucose oxidase catalyzed glucose oxidation and oxidase nanozyme catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB) colorimetric oxidation. As a proof of concept, Co-Nx sites on porous carbon (Co-Nx/PC) derived from ZIF-67 was selected as the oxidase nanozyme with O 2 -sensitive nature, which can activate O 2 to produce 1 O 2 for TMB colorimetric oxidation. In the presence of glucose, the competitive reaction of glucose oxidase catalyzed glucose oxidation occurs, which will obviously inhibit the Co-Nx/PC catalyzed TMB colorimetric oxidation to construct method for glucose detection. The usage of the same reactant O 2 and the production of suppressive H 2 O 2 cause a dual effect to this inhibition. In addition, the available pH range of Co-Nx/PC overlaps with that of glucose oxidase, promising a one pot reaction . The proposed method with Co-Nx/PC as oxidase nanozyme based on one-step competitive strategy for glucose detection possesses high detection efficiency with convenience (one-pot), rapidness (total reaction time of 10 min) and sensitivity (LOD of 0.31 μM) all promised, which is superior among the methods based on two-step one-pot or two-pot cascade strategy. The strategy can be successfully applied into the blood glucose detection in human serums with satisfactory results. Also, the strategy can be scalable to other oxidase nanozyme like Mn 3 O 4 .
研究领域:
生物化学
·
医学检测
·
纳米技术
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DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Lili Liu,Chen Wang,Luxin Zhao,Yayun Xiao,Weiwei Fang,Lanling Zhao,Faxing Wang,Yuping Wu
The practical development of Li-O 2 batteries (LOBs) urgently needs to explore robust cathode catalysts to boost the sluggish Li 2 O 2 reaction kinetics and parasitic reactions despite their theoretically high specific energy. Profound understanding of the cathode properties and the battery performance is rather critical in developing rational-designed electrocatalysts. In this study, a Co-N x /Co (111) decorated N-doped hierarchical carbon framework (Co-N x /Co@NHCF) is proposed as an efficient cathode in LOBs. Spectroscopic analysis coupled with experimental results suggests that the Co-N x /Co (111) catalytic center can significantly reduce the battery overpotential, and meanwhile, the hierarchical carbon framework ensures rapid mass transportation and provides sufficient space to accommodate Li 2 O 2 deposition. Density functional theory calculations reveal that the incorporated Co (111) facet can effectively regulate the electronic distribution of N-carbon, optimize the adsorption of desirable intermediates, and eventually facilitate oxygen reduction reaction/oxygen evolution reaction kinetics. As expected, the Co-N x /Co@NHCF catalyzed LOBs deliver a high discharge/charge capacity of 6.15/ 6.22 mAh cm −2 with a columbic efficiency of 98.9%, along with a high rate cycling of 700 h at 0.3 mA cm −2 . This work provides valuable instruction for the rational design of efficient catalysts for high-performance LOBs via optimization of the crystal structure and the adsorption of intermediates.
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DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 32
·期 12
·e4570
·
IF 3.581
Xiaobin Dong,Chaoyue Zhao,Qingxin Guan,Wei Li,Xiufang Xu
Industrial production of vinyl chloride through acetylene hydrochlorination is a dominating technique in coal-rich areas, but its development is severely restricted by the use of toxic mercury chloride (HgCl 2 ) catalyst. Inspired by the fact that doped carbon materials active in acetylene hydrochlorination often have good performance in the oxygen reduction reaction, a series of cobalt and nitrogen co-doped porous carbon catalysts prepared by pyrolysis of bimetallic ZIFs based on ZIF-8 and ZIF-67 under N 2 were applied in acetylene hydrochlorination. The catalytic activities of the co-doped catalysts varied with Co addition, and the highest acetylene conversion could be up to 83% with a space velocity of 2.6 ml g −1 min −1 at 220°C when a small amount of cobalt was introduced. Results of several characterizations confirmed the existence of Co–N x in the co-doped carbons, pointing out that this coordination structure makes the catalysts have better ability to adsorb and activate C 2 H 2 . Density functional theory calculation finally proved that C atom adjacent to the N atom in Co–N 4 structure is the primary active site in co-doped catalysts with high activity. We also conclude that the decreased N content caused by Co 2 N decomposition and the coordination structure change of Co–N x should be responsible for the gradually worsening performances of the carbon catalysts with further Co addition. Our study provides a new route for improving the performance of N-doped carbon material in acetylene hydrochlorination and thus enhances its potential for practical application.
研究领域:
化学工程
·
催化材料
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产品关联
DOI
高影响因子
ACS Nano
·
2021
·
IF 15.881
Ting Huang,Yingjie Sun,Jianghua Wu,Jia Jin,Chaohui Wei,Zixiong Shi,Menglei Wang,Jingsheng Cai,Xing-Tao An,Peng Wang,Chenliang Su,Ya-yun Li,Jingyu Sun
Although lithium–sulfur (Li–S) batteries have long been touted as next-generation energy storage devices, the rampant dendrite growth at the anode side and sluggish redox kinetics at the cathode side drastically impede their practical application. Herein, a dual-functional fibrous skeleton implanted with single-atom Co–Nx dispersion is devised as an advanced modificator to realize concurrent regulation of both electrodes. The rational integration of single-atomic Co–Nx sites could convert the fibrous carbon skeleton from lithiophobic to lithiophilic, helping assuage the dendritic formation for the Li anode. Meanwhile, the favorable electrocatalytic activity from the Co–Nx species affording a lightweight feature effectively enables expedited bidirectional conversion kinetics of sulfur electrochemistry, thereby inhibiting the polysulfide shuttle. Moreover, the interconnected porous framework endows the entire skeleton with good mechanical robustness and fast electron/ion transportation. Benefiting from the synergistic effects between atomically dispersed Co–Nx sites and three-dimensional conductive networks, the integrated Li–S full batteries can achieve a reversible areal capacity (>7.0 mAh cm–2) at a sulfur loading of 6.9 mg cm–2. This work might be beneficial to the development of practically viable Li–S batteries harnessing single-atom mediators.
研究领域:
材料科学
·
能源存储与转换
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DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Mingzhu Wang,Shuyu Yue,Xingyun Zhao,Yaoyan Wu,Yaohui Zhang,Yaqian Dong,Tiehua Ma
Developing highly efficient and durable trifunctional electrocatalysts is essential for advancing technologies related to water splitting, oxygen reduction, and hydrogen storage, which are critical for energy conversion and storage. In this study, we encapsulated Co-MOFs on the surface of Mo2C hollow spheres and achieved the Co@NC/Mo2C composite material through high-temperature annealing. In the optimal catalyst, Co@NC/Mo2C-0.1, Co@NC nanosheets were uniformly distributed on the Mo2C hollow spheres, and the BET surface area was well maintained. Compared to Co nanoparticles, Co-Nx in Co@NC/Mo2C-0.1 exhibited a greater modulation effect on the electronic structure of Mo2C. Density functional theory (DFT) calculations showed that the Co@NC/Mo2C heterostructure effectively lowered the energy barrier for the hydrogen evolution reaction (HER) on Mo2C and enhanced the performance of the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) through electronic coupling. Specifically, for Co@NC/Mo2C-0.1, at a current density of 10 mA cm–2, the half-wave potential for ORR was 0.86 V, the overpotential for OER was 349 mV, and the overpotential for HER was 158 mV. Additionally, this catalyst exhibited exceptional stability across all three reactions, making it an ideal candidate for sustainable energy technologies.
研究领域:
材料科学
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电化学
·
能源技术
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Jiahui Xu,Jia-qi Bai,Wenjie Si,Yunhai Zhang,Jiazhao Tan,Mengdie Cai,Qin Cheng,Song Sun
Non-noble metals have attracted worldwide attention for the catalytic hydrogenation of halonitrobenzene due to their high activity, low price, and abundance on Earth. However, the construction of effective and stable non-noble-metal catalysts for the selective hydrogenation of halonitrobenzene to haloaniline by a simple method remains challenging. Herein, we report a facile one-pot method for the synthesis of N,S-co-doped mesoporous carbon-supported non-noble-metal catalysts through carbonization of a mixture of metallic precursors and 2-aminothiazole in molten ZnCl2. The prepared Co-NSPC catalyst showed excellent activity and selectivity with a turnover frequency of 84.4 h–1 in the hydrogenation of p-chloronitrobenzene to p-chloroaniline. Furthermore, Co–Nx was found to be the main active site for this reaction on the basis of characterization and experimental data, and the introduction of S promoted the formation of Co–Nx sites. Moreover, the Co-NSPC-800 catalyst can be reused at least four times and applied to the hydrogenation of 10 kinds of halogenated nitrobenzenes with excellent selectivity.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yang Li,Yihao Jing,Yiguo Zhao,Wentao Li,Jing Li,Yuqing Song,Yue Yang,Tingting Feng,Gen Peng,Zhenpeng Huang,Ting Yang,Qi Zhou
In this study, novel Co-embedded hollow N -doped carbon polyhedrons, derived from ZIF-8@ZIF-67 core–shell structure, were synthesized and used for activating peroxymonosulfate (PMS) towards efficient bisphenol A (BPA) degradation. The contents of different N species, especially Co-N x and graphitic N sites, were tuned by different calcination temperatures (800, 900, and 1000 °C). Characterization results demonstrated that hollow polyhedron with high graphitization degree and abundant porosity anchored numerous Co nanoparticles, which could enhance the catalytic performance. Compared to other as-prepared catalysts, Co/HNCP-900 (pyrolyzed at 900 °C) showed a more outstanding performance of PMS activation towards BPA degradation, and 95.1 % of BPA (20 mg/L) could be removed within 3 min. Abundant Co-N x sites were a critical factor to induce the reaction process. Based on trapping, radical scavenger, and electrochemical analysis experiments, a nonradical process (singlet oxygen and direct electron transfer) was proposed to play the dominant role in BPA degradation. Benefiting from the nonradical process, BPA degradation efficiency almost remained stable either in a wide pH range (2.5–8.0) or in the presence of coexisting ions and natural organic matter. The findings of this study will elucidate a new opportunity for improving environmental remediation.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jian Tang,Yujie Wang,Jun Ma,Yujie Chen,Ming Chen
In this study, we selected rice straw, wheat straw and corn cob as raw materials to successfully prepare cobalt-nitrogen co-doped biomass-based carbon nanotubes composites (BM@CoNCNTs) with Co-N x sites highly dispersed on porous biochar carrier, which could effectively activate peroxymonosulfate (PMS) to remove tobacco mosaic virus (TMV) in water. Particularly, BM@CoNCNTs-CC, with its confined carbon nanotubes and high-density Co-N x sites, enhanced the Co 2+ /Co 3+ cycle and direct adsorption of PMS to generate Co(IV)=O and 1 O 2 , playing a dominant role. This led to the effective disruption of TMV coat protein and degradation of its genome within 5 min, achieving up to 6 log 10 removal efficiency. Additionally, BM@CoNCNTs-CC/PMS system maintained efficient catalytic removal performance even in complex water matrices (river water and tap water). Overall, our research not only elucidates the production of efficient biomass-based catalysts for environmental remediation, but also highlights the application potential of biomass-based carbon nanotubes composites enriched with Co-N x sites.
研究领域:
环境科学
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纳米技术
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水处理
·
病毒学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meiling Liu,Liping Wang,Qilong Fan,Ningning Xiao,Zhiwen Chen,Yingying Dong,Chuanliang Zhao,Yongxia Sun,Xing Xu,Wendong Wang
Nitrogen (N)-doping has been reported effective to reinforce catalysis in advanced oxidation processes (AOPs) due to the formation of N-related active sites. Although several documents have reported that transition metal-nitrogen (metal-N x ) sites could work as reactive centers, the catalytic mechanism was hardly elucidated. In this study, N-doped cobalt oxide (N-CoO x ) was initiatively prepared via calcination in ammonia atmosphere to construct cobalt-nitrogen (Co-N x ) sites. The emergence of Co-N x sites effectively improved peroxymonosulfate (PMS) activation efficiency (above 5.8 times), leading to higher pollutant decomposition rate (95.8 % at 30 min) and kinetics constant (above 4.1 times). N introduction changed main facets of material and elevated adsorption energy (E ads ) (from −1.81 eV to −3.71 eV) between catalyst and PMS. Co atoms at Co-N x sites could donate larger quantity of electrons (from 1.088 e to 1.583 e) to PMS, therefore, contributed to stretching and breaking O–O bonds of PMS molecules to form reactive species. As a result, both radical and electron transfer pathway (ETP) were enhanced in the oxidation processes. Ultimately, the catalytic membrane coated with N-CoO x maintained 100 % treatment towards continuous antibiotic wastewater at environmentally relevant concentration (μg/L), realizing purification as well as separation of catalyst. This work systematically elaborates the superiority of Co-N x sites and unravels the underlying mechanism to inspire further study to metal-N x tailored catalysis.
研究领域:
环境科学
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催化
·
材料科学
·
水处理
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DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Luo Huihui,Tian Shuainan,Liang Hongliang,Wang He,Gao Shuang,Dai Wen
The cleavage and functionalization of C–S bonds have become a rapidly growing field for the design or discovery of new transformations. However, it is usually difficult to achieve in a direct and selective fashion due to the intrinsic inertness and catalyst-poisonous character. Herein, for the first time, we report a novel and efficient protocol that enables direct oxidative cleavage and cyanation of organosulfur compounds by heterogeneous nonprecious-metal Co-N-C catalyst comprising graphene encapsulated Co nanoparticles and Co-Nx sites using oxygen as environmentally benign oxidant and ammonia as nitrogen source. A wide variety of thiols, sulfides, sulfoxides, sulfones, sulfonamides, and sulfonyl chlorides are viable in this reaction, enabling access to diverse nitriles under cyanide-free conditions. Moreover, modifying the reaction conditions also allows for the cleavage and amidation of organosulfur compounds to deliver amides. This protocol features excellent functional group tolerance, facile scalability, cost-effective and recyclable catalyst, and broad substrate scope. Characterization and mechanistic studies reveal that the remarkable effectiveness of the synergistic catalysis of Co nanoparticles and Co-Nx sites is crucial for achieving outstanding catalytic performance.
研究领域:
催化
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有机化学
·
材料科学
·
环境化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2023
·
IF 4.1
Peipei Liu,Meiling Fan,Yapeng Cheng,Hongfei Pan,Jin Liu,Haining Zhang
Porous carbon materials with nitrogen-coordinated transition metal active sites have been widely regarded as appealing alternatives to replace noble metal catalysts in oxygen-based electrochemical reaction activities. However, improving the electrocatalytic activity of transition-metal-based catalysts remains a challenge for widespread application in renewable devices. Herein, we use a simple one-step pyrolysis method to construct a Co nanoparticles/Co–Nx-decorated carbon framework catalyst with a near-total external surface structure and uniform dispersion nanoparticles, which displays promising catalytic activity and superior stability for oxygen reduction reactions in both alkaline and neutral electrolytes, as evidenced by the positive shift of half-wave potential by 44 and 11 mV compared to 20% Pt/C. Excellent electrochemical performance originates from highly accessible Co nanoparticles/Co–Nx active sites at the external surface structure (this is, exposing active sites). The thus-assembled liquid zinc–air battery using the synthesized electrocatalyst as the cathode material delivers a maximum power density of 178 mW cm–2 with an open circuit potential of 1.48 V and long-term discharge stability over 150 h.
研究领域:
电化学
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材料科学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）