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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Molten salt induced formation of chitosan based carbon nanosheets decorated with CoNx for boosting rechargeable Zn-air batteries

Qiusheng Zhou,Yuan Tian,Mingyuan Wang,Shuangying Lei,Chuanyin Xiong

The earth-abundant, low-cost, and efficient oxygen electrode materials offer a potential opportunity to satisfy the large-scale production and application of metal-air batteries. Herein, a molten salt-assisted strategy is developed to anchor transition metal-based active sites via in-situ confining into porous carbon nanosheet. As a result, a chitosan-based porous nitrogen-doped nanosheet decorated with the well-defined CoN x (CoN x /CPCN) was reported. Both structural characterization and electrocatalytic mechanisms demonstrate a prominent synergetic effect between CoN x and porous nitrogen-doped carbon nanosheets forcefully accelerates the sluggish reaction kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Interestingly, the Zn-air batteries (ZABs) equipped with CoN x /CPCN-900 as an air electrode shows outstanding durability for 750 discharge/charge cycles, a high power density of 189.9 mW cm −2 , and a high gravimetric energy density of 1018.7 mWh g −1 at 10 mA cm −2 . Furthermore, the assembled all-solid cell displays exceptional flexibility and power density (122.2 mW cm −2 ).

研究领域: 材料科学 · 电化学 · 能源存储与转换
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Cytosine-Co assemblies derived CoNx rich Co-NCNT as efficient tri-functional electrocatalyst

Yu Wang,Honghao Yu,Liangkui Zhu,Zhiqiang Shi,Runwei Wang,Zongtao Zhang,Shilun Qiu

Carbon-metal composites are promising multifunctional electrocatalysts , but it is still challenging to prepare carbon-metal composites with tunable structure and strong metal-carbon interactions. Here, we present a unique gas-foaming assembly strategy to prepare cytosine-Co chelate derived Co and N codoped carbon nanotube (Co-NCNT). The structure for Co-NCNTs could be easily controlled by regulating cytosine-Co coordination or the carbonization temperature. The optimal Co-NCNT possesses homogeneous distributed NCNTs (10 nm), CoO x (5 nm) and CoN x moieties to synergistically boost electrochemical processes, and offer mesoporous nanosheet architecture to guarantee fast mass migrate and electron transfer . As a result, Co-NCNT shows remarkable ORR performance (onset potential of 0.93 V in 0.1 M KOH electrolyte) along with significant OER and HER activity. More important, it was found that CoN x moieties are responsible for the remarkable electrocatalytic activity in Co-NCNTs, because CoN x could alter active center, enhance metal-carbon synergy, decrease interfacial resistance and reinforce the strength of composites. Therefore, this paper not just demonstrates an advanced multi-functional electrocatalyst, but could also give deep understanding on the designing of multifunctional electrocatalysts.

CAS / MDL: 71-30-7
研究领域: 材料科学 · 电化学
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JOURNAL OF THE ENERGY INSTITUTE · 2025 · IF 6.2

Catalytic hydrofining of thermal dissolution-derived liquefied oil from Dongming lignite into cyclanes-rich liquid fuel over Co-CoNx@C650

Hao-Dong An,Guang-Hui Liu,Yan-Jun Li,Ling-Zhi Tuo,Yu-Hong Kang,Zhi-Ping Wang,Yong Gao,Chen Shi,Yun-Yan Gao,Xian-Yong Wei

Hydrofining of low-grade lignite liquefied oils into high-density liquid fuels is a critical pathway for their value-added utilization. However, abundant condensed aromatic rings (ARs) and O atoms in such crude oils pose significant challenges for secondary upgrading, particularly in achieving concurrent AR hydrogenation and hydrodeoxygenation in one-pot to produce alkyl cyclanes. In view of this, Co-CoN x @C 650 was constructed by a cascade preparation strategy consisting of in-situ co-pyrolysis and NH 3 nitridation. It has highly dispersed Co-CoN x dual-sites and carbon substrate with abundant defects/vacancies, and exhibits good performance in AR hydrogenation and hydrodeoxygenation. In addition, this catalyst can effectively activate H 2 and promote the synergistic transfer of H ··· H, δ+ H ··· H δ− , and H · . Good accessibility, cyclic stability, and renewability make it suitable for the hydrogenation of medium/large-sized molecules such as naphth-2-ol and aryl ethers into cyclanes. The liquefied oil (SP TD ) from Dongming lignite thermal dissolution in n -hexane is rich in aromatics (76.1 %), while refined oil (CHSP TD ) from catalytic hydrofining over Co-CoN x @C 650 is rich in saturated hydrocarbons (91.7 %), especially alkyl cyclanes (69.8 %). The efficient conversion of aromatic-oxygenated moieties demonstrated by Co-CoN x @C 650 provides a new solution for converting low-grade lignite liquefied oils into value-added cyclanes-rich liquid fuels.

研究领域: 能源化学 · 催化材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Controlled synthesis of FeNx-CoNx dual active sites interfaced with metallic Co nanoparticles as bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries

Yi-jin Wu,Xiao-hong Wu,Teng-xiu Tu,Peng-fang Zhang,Jun-tao Li,Yao Zhou,Ling Huang,Shi-gang Sun

Efficient bifunctional oxygen electrocatalysts are essential for high-performance rechargeable Zn-air batteries (rZABs). Herein, a porous hollow carbon nanoshell (H-Co@FeCo/N/C) in which FeN x and CoN x metal sites are atomically dispersed and interfaced intimately with metallic Co nanoparticles was derived from pyrolysis of polydopamine-coated ZnCo-ZIFs adsorbed with Fe 3+ ; the chemical interactions among different organic and metal species during the polymer-coating process was inverstigated; their role in regulating the size of the Co nanoparticles, the structure of the hollow carbon nanoshell and the formation of the FeN x -CoN x dual active sites was revealed. The H-Co@FeCo/N/C showed superior bifunctional oxygen electrocatalytic activity (Δ E  = 0.698 V) and mass activity of 6.8 A g cat. −1 at 0.9 V, outperforming the commercial Pt/C/RuO 2 catalysts or the Fe/N/C or Co/N/C counterparts. When assembled for rZABs, the H-Co@FeCo/N/C cathode displayed a long cycle life of 200 h ( E gap of about 1.0 V@10 mA cm -2 ).

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Enhanced electron transfer-based nonradical activation of peroxymonosulfate by CoNx sites anchored on carbon nitride nanotubes for the removal of organic pollutants

Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu

The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.

研究领域: 环境科学 · 催化 · 水处理 · 材料科学
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CATALYSIS TODAY · 2022 · IF 6.562

High-density atomically dispersed CoNx catalysts supported on nitrogen-doped mesoporous carbon materials for efficient hydrogenation of nitro compounds

Xiangru Wei,Zeyu Hu,Cancan Li,Yali Zhang,Xianglin Xie,Hao Wang,Zhangxiong Wu

Carbon supported atomically dispersed transition metal–nitrogen (MN x ) catalysts are promising for catalysis. Synthesis of such catalysts with high densities of MN x sites is an important task. In this work, a facile and scalable method by combining freeze drying and hard templating is presented for the synthesis of N-doped mesoporous carbon supported high-density and exclusive CoN x sites (denoted as CoN x -NMCs). The influences of the drying method (freeze drying and regular drying) on the aggregation of the silica pore forming agent, the precursor and metal species and the properties and performances of the resulted catalysts are investigated. The strong Co 2+ /histidine and silica/histidine interactions and the homogeneous distribution of the SiO 2 nanoparticles for precursor physical isolation are essential to inhibit metal aggregation, sustain N dopant and generate high densities of CoN x sites. The CoN x -OMCs possess high surface areas (440–630 m 2 /g), uniform mesopores (~ 7 nm), high N contents (2.54–17.84 wt%) and abundant CoN x sites with high single cobalt atom loadings up to 1.7 wt%. The representative catalyst delivers outstanding catalytic performances for hydrogenation of a series of nitro compounds into amines with excellent conversions and selectivities and a high stability with H 2 as the reducing agent and water as the solvent. A series of control experimental results clearly reveal the critical role of the CoN x sites for the chemoselective hydrogenation and clarify the influences of the properties of the catalysts on their performances. The work may provide a general approach and some insight for the development of atomically dispersed MN x catalysts with a high metal atom utilization efficiency for the purpose of various catalytic applications.

CAS / MDL: 141-78-6
研究领域: 催化 · 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Bimetallic and nitrogen co-doped biochar for peroxymonosulfate (PMS) activation to degrade emerging contaminants

Shizong Wang,Jianlong Wang

In this study, the bimetallic and nitrogen co-doped biochar was prepared for peroxymonosulfate (PMS) activation to degrade emerging contaminants. Compared to single metal-doped biochar, bimetallic-doped biochar showed much higher catalytic activity. Iron and cobalt co-doped biochar (FeCo-BC) exhibited higher catalytic activity than iron and copper co-doped biochar (FeCu-BC). When FeCo-BC was used for PMS activation, sulfamethoxazole (SMX) could be completely removed within 10 min, with the degradation rate of 0.749 min −1 , which was 2.3 and 69.4 times higher than that of Fe-BC (0.333 min −1 ) and Co-BC (0.0108 min −1 ), respectively, demonstraing the synergistic effect of bimetallic co-doping. Meanwhile, the SMX mineralization efficiency reached 57.1 %. In the system of FeCo-BC/PMS, multi reactive species produced, in which hydroxyl radicals, sulfate radicals and high-valent metal-oxo mainly contributed to SMX degradation. The superior catalytic activity of FeCo-BC was attributed to the configuration of FeNx-CoNx. In five consecutive experiments, FeCo-BC showed good catalytic activity and stability. This study provides a way to the rational design of high efficient and stable PMS catalyst, which could be used in Fenton-like reaction to remove the emerging organic contaminants.

研究领域: 环境科学 · 催化材料 · 污染治理
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Optimizing the electronic structure of CoNx via coupling with N-doped carbon for efficient electrochemical hydrogen evolution

Peiyun Zhou,Rushuo Li,Junjun Lv,Gongchi Zhao,Xiaowei Zhang,Xiubing Huang,Yunfeng Lu,Ge Wang

Transition metal nitrides (TMNs) have been regarded as an excellent class of electrocatalysts for hydrogen evolution reaction (HER), but there is still huge room for improvement. In this work, cobalt nitride (CoN x ) coupled with N-doped carbon (N C) and supported by nickel foam (NF) is designed as an efficient HER electrocatalyst (NF/CoN x @N C). The introduction of N C can not only optimize the electronic structure of CoN x to boost the intrinsic activity, but also enhance the electronic conductivity and stability of the catalyst. As a result, NF/CoN x @N C exhibits excellent HER performance. On the one hand, it only needs an overpotential of 69 mV to deliver a current density of 20 mA cm −2 in 1.0 mol/L KOH, far better than that of CoN x (182 mV). On the other hand, the electronic conductivity and stability of the catalyst can be significantly enhanced after the introduction of N C. This work has done successful material design with the goal of enhancing the intrinsic activity, electronic conductivity, and stability, which has certain reference and guiding significance for the design of novel transition metal-based electrocatalysts.

研究领域: 材料科学 · 电化学
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Nanoscale · 2017 ·Vol. 9 ·期 24 ·8341-8348 · IF 7.367

Architecture of CoNx single clusters on nanocarbon as excellent oxygen reduction catalysts with high-efficient atomic utilization

Ting He,Hui Xue,Xiaojuan Wang,Shuanghua He,Yulai Lei,Yuyuan Zhang,Rujuan Shen,Yi Zhang,Juan Xiang

A new strategy to fabricate CoNx single cluster supported nanocarbon catalysts (C/P/2Co600) with enhanced atomic utilization towards the oxygen reduction reaction (ORR) is reported. N-Coordination protection and low-temperature pyrolysis are the two key factors for the formation of CoNx single clusters on nanocarbon supports. Morphological and structural identification confirmed the simultaneous anchoring of homo-dispersed CoNx single clusters and N-doping on the nanocarbon under relatively mild thermal treatment conditions. Expectedly, the obtained single cluster catalyst with a trace amount of metal atoms exhibited excellent ORR performance including a positive half-wave potential (0.846 V), a high mass activity (0.98 A mgCo−1, ampere per milligram of cobalt) and outstanding chemical durability after 8000 potential cycles. We believe that our findings provide a new route for the rational design of low-cost and highly active ORR catalytic materials.

研究领域: 材料科学 · 催化化学
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 10 ·5580-5592 · IF 14.511

Synergistic effect of Co catalysts with atomically dispersed CoNx active sites on ammonia borane hydrolysis for hydrogen generation

Pui-Ching Poon,Yuanhao Wang,Weiqun Li,Dawson Wai-Shun Suen,William Wai Yan Lam,Denise Zi Jing Yap,B. Layla Mehdi,Jun Qi,Xiao-Ying Lu,Eugene Yin Cheung Wong,Chunzhen Yang,Chi-Wing Tsang

The development of low-cost, highly efficient and durable catalysts is the key to the practical use of ammonia borane as a promising storage material for on-board hydrogen production. Atomically dispersed metal supported catalysts not only maximize the efficiency of metal utilization, but they can also act as a robust support for metal nanoparticles. Herein, we report a facile synthesis of a type of carbon nanotube that consists of both Co nanoparticles and atomically dispersed cobalt single-atoms by direct carbonization of a mixture of cobalt-containing precursors and melem-C3N4. Our results suggested that Co nanoparticles were successfully embedded in the layers of graphitic carbon to effectively prevent them from aggregation and loss of catalytic activity. In addition, the Co single atoms greatly lowered the adsorption barriers of water molecules onto the catalysts for fast hydrolysis of ammonia borane. Interestingly, it was found that when the ratio of Co to melem-C3N4 was 1 : 33.3, the best reactivity and stability towards ammonia borane hydrolysis were achieved. The highest specific hydrogen generation rate can reach up to 7833 mLH2 gCo−1 min−1 at 40 °C, which far exceeded most of the non-noble metal catalysts for ammonia borane hydrolysis to date. The durability of the catalyst was successfully maintained for 40 cycling tests and no obvious decay was observed. The current study presents an example of how nanoparticles and single-atoms can be synergistically exploited for heterogeneous catalysis applications.

研究领域: 催化化学 · 材料科学 · 能源研究
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Porous carbon nanosheets integrated with graphene-wrapped CoO and CoNx as efficient bifunctional oxygen electrocatalysts for rechargeable zinc-air batteries

Chang Ma,Binji Zhu,Yue Wang,Shuwen Ma,Jingli Shi,Xiangwu Zhang,Yan Song

The development of advanced bifunctional oxygen electrocatalysts for the oxygen reduction reactions (ORR) and oxygen evolution reactions (OER) is crucial for the practical application of zinc-air batteries (ZABs). Herein, porous carbon nanosheets integrated with abundant graphene-wrapped CoO and CoNx (CoO/CoNx-C) were successfully fabricated through a simple one-step pyrolysis. With convenient porous channel and large accessible surface, abundant CoO/CoNx species and graphene wrapping structure, CoO/CoNx-C exhibited a half-wave potential of 0.844 V in ORR and an overpotential of 384 mV (@10 mA cm −2 ) in OER in the alkaline environment and presented a negative shift of 9 mV in ORR after 8000 cycles and positive shift of 19 mV in OER after 2000 cycles. Electrochemical acid-washing and comparison analysis revealed that the ORR activity mainly originated from CoO nanoparticles, while CoNx species were greatly responsible for OER catalysis. Furthermore, the as-prepared CoO/CoNx-C endowed the rechargeable liquid and solid ZABs with superior power density (161 mW cm −2 for liquid ZABs and 137 mW cm −2 for solid ZABs) and long-term stability (stable in 1000 h charge/discharge tests) compared to commercial catalysts. This work provides a feasible strategy for cobalt/carbon hybrid materials as advanced bifunctional electrocatalysts for ZABs.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

In Situ Fabrication of Defective CoNx Single Clusters on Reduced Graphene Oxide Sheets with Excellent Electrocatalytic Activity for Oxygen Reduction

Ting He,Xiaojuan Wang,Huiqiong Wu,Hui Xue,Peng Xue,Jing Ma,Minli Tan,Shuanghua He,Rujuan Shen,Lunzhao Yi,Yi Zhang,Juan Xiang

A facile one-step strategy for anchoring defective CoNx single clusters on partly reduced graphene oxide (RGO) is constructed to significantly improve the catalytic performance of non-noble metal complexes toward oxygen reduction reaction (ORR). Sequent loading with trace amounts of metal-free porphyrin and Co2+ in RGO can dramatically enhance both the half-wave potential and the peak current density. Intriguingly, the RGO/P/2Co single cluster exhibits the best ORR catalytic performance with the half-wave potential of 0.834 V, extremely approaching that of commercial Pt/C (0.836 V). This half-wave potential surpasses most of the reported half-wave potentials of RGO supported non-noble metal ORR catalysts through low-temperature synthesis. Furthermore, the as-prepared RGO/P/2Co delivers a peak current density of 1.3 times higher than that of Pt/C at the same loading, together with a high mass activity of 2.76 A mgCo–1. During the durability test, a cathodic current loss less than 10% is recorded after 8000 continuous potential cycles. Insights into this successful example will be conducive to the development of elegant routes for constructing metal nitrogen (MN)-based ORR catalysts with high efficiency, outstanding stability, and excellent selectivity.

研究领域: 材料科学 · 电化学
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