Journal of CO2 Utilization
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2022
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IF 8.321
Jian-Lei Qi,Qin-Qin Xu,Dan Zhou,Jian-Zhong Yin
Supported single-atom catalytic materials (SACMs) have aroused extensive interest due to their remarkable properties. Herein, a novel method was proffered to prepare Co-NC SACMs using custom-designed N-doped carbon (NC) as support, CoCl 2 as the precursor in supercritical CO 2 with appropriate co-solvent. It was found that when ethanol was used as co-solvent, nanoparticles were obtained while only Co single-atom was obtained when N, N-Dimethylformamide (DMF) was used as co-solvent. Both the theoretical loading and the deposition time influenced the Co loading a lot, and the maximum Co loading was as high as 1.71 wt%. Strong acid, strong alkali, corrosive solvent, and high-temperature treatment were avoided in the whole process. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray photoelectron spectroscopy (XPS), Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES), and Energy Dispersive X-ray spectroscopy (EDX) were conducted to confirm the existence and uniform distribution of Co atoms over the N-doped carbon materials. The conversion rate of 90.0% and selectivity of 86.0% were obtained for the solvent-free selective oxidation of benzyl alcohol to benzaldehyde at 70 °C and 1 h using the Co-NC SACMs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Yuhan Long,Songrong Li,Peizhen Yang,Xi Chen,Wenhao Liu,Xuesong Zhan,Cheng Xue,Dongfang Liu,Wenli Huang
MOF-derived metal-carbon composite catalyst was an alternative high-efficient catalyst for activating peroxymonosulfate (PMS). In this study, a novel cobalt-carbon-nitrogen doped composite catalyst with honeycomb porous structure (Co-HPNC) was obtained through a simple strategy consisting of three steps: self-growth of ZIF-67 on the SiO 2 core, pyrolysis, and NaOH etching away SiO 2 core. The Co-HPNC exhibited an outstanding catalytic performance (98.1% in 10 min) to activate PMS for acid orange 7 (AO7) degradation. The observed reaction kinetic constant (0.4319 min −1 ) was 2.64 times superior to that of the unmodified Co/NC catalysis system (0.1636 min −1 ). In the meantime, the catalyst demonstrated a high PMS activation capacity over a wide pH range of 3–11 and strong adaptability to the high concentration of inorganic anions (Cl - , SO 4 2- , and CO 3 2– ). After being recycled three times, the removal efficiency could still reach 92.7% in 25 min. The quenching tests and EPR spectrum illustrated the existence of radical and non-radical pathways, in which singlet oxygen was dominant during the degradation process. It was hypothesized that Co(0)/Co(Ⅱ)/Co(Ⅲ), pyridinic-N and pyrrolic-N contributed to the generation of hydroxyl and sulfate radicals, while C=O functional group and graphitic-N were catalytic sites for singlet oxygen. Finally, the radical electrophilic attacking sites of AO7 were calculated by the density functional theory (DFT), and the degradation routes of AO7 were speculated by GC–MS. The toxicity test illustrated that the Co-HPNC/PMS system was an environmental-friendly technology for AO7 degradation. The prepared Co-HPNC with a unique honeycomb porous structure presents a novel synthesis route for MOF-derived catalyst applied in the PMS activation system for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Dan Xu,Jianfeng Li,Boyang Li,Huacheng Zhao,Hanghang Zhu,Jinfang Kou,Fengwei Zhang,Zhengping Dong,Jiantai Ma
The sustainable catalytic transformation of alcohols to high value-added fine chemicals is a significant and challenging research topic. Herein, a set of nitrogen-doped carbon encapsulated Co-based catalysts (Co-Co 3 O 4 @NC-T) were prepared by using low-cost dicyandiamide, glyoxal and cobalt nitrate as precursors. The obtained catalysts were utilized for the selective oxidation of alcohols to high value-added esters and carboxylic acids with air as the oxygen source and displayed wide applicability for the oxidation of both aromatic and aliphatic alcohols. Based on the controlled experiments, the protective effect of N-doped carbon structure and the synergistic effect between Co core and Co 3 O 4 species guaranteed the high reaction conversion and selectivity. Benefitting from heterogeneity and magnetism of the catalyst, it can be easily recycled and reused for long-term stability. Reasonable mechanisms of selective oxidation reaction were proposed through EPR analysis and controlled experiments. The present work provides a facile strategy for potential large-scale preparation of heterogeneous catalyst for sustainable and green catalytic transformations.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Manfen Liang,Yu Liu,Jie Zhang,Fangyuan Wang,Zhichao Miao,Lechen Diao,Jinglin Mu,Jin Zhou,Shuping Zhuo
The electrochemical CO 2 reduction reaction (CO 2 RR) that transforms CO 2 to CO has attracted great interest. Transition metal nanoparticles encapsulated in nitrogen-doped carbon (M@NC) catalysts exhibit outstanding catalytic performance. However, the role of metal and N species in M@NC catalysts remains unclear. In this work, Co@C, Co@NC, Ni@C, and Ni@NC catalysts were achieved and employed in CO 2 RR. The Ni@NC catalyst exhibits an industry level current density of 220 mA cm −2 and a high Faradaic efficiency of 98% for CO production at − 0.87 V vs. RHE for 100 h. In addition, the N species, especially the pyrrolic-N in the shell of Ni@NC material provide active sites for adsorbing and activating CO 2 molecules, and metal nanoparticles improve the electronic structure of N species, thereby decreasing their ability for radical attack (*COOH, *CO, and *H). Consequently, this work can guide the design of M@NC catalyst for CO 2 RR to CO.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Weiping Xiao,Daqiang Yan,Qin Zhao,Danil Bukhvalov,Xiaofei Yang
Developing the Pt-based intermetallic nanoparticles could accelerate the sluggish kinetic of oxygen reduction reaction, while it remains a great challenge to explore efficient synthesis strategies enhancing thermal stabilities and electrocatalytic properties. This work employed the metal-support coupling strategy to construct the Pt 3 Co/CoNC hierarchical nanostructure , where the well-dispersed atomically ordered Pt 3 Co nanoparticles were anchored on the Co-NC sites. Physical structure analysis combined with density functional theory calculations demonstrated the strong coupling effect between Pt and surrounding Co-NC sites, which could weaken the activation energy to break O-O bonds and enhance the intrinsic activity and stability of Pt. Hence, the Pt 3 Co/CoNC exhibited the optimized ORR activities with the half-wave potentials of 0.97 V in KOH solution and displayed the peak power density of 187 mW cm −2 as the cathode of Zn-air battery. This metal-support coupling strategy can be further generalized and improved to synthesize other Pt-based catalysts with efficient electrocatalytic properties.
研究领域:
材料科学
·
电化学
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ChemSusChem
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2024
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IF 7.5
Bin Zhu,Qiuge Wang,Jinggang Wang,Xiao Yu,Jian Zhang,Chunlin Chen
Graphical The nitrogen-doped-carbon encapsulated cobalt (Co@NC) chainmail nanowires were synthetized for the electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) from 2,5-bis(hydroxymethyl)furan (BHMF). The Co@NC on Ni foam achieved 97.9 % conversion of BHMF, yielding 93.3 % FDCA at 1.475 V vs. RHE. The superior electrochemical performance of Co@NC/NF can be attributed to its large electrochemically active surface area and excellent kinetic parameters. 2,5-Furandicarboxylic acid (FDCA) has emerged as an important bio-based furanic compound, which has broad application prospects in renewable energy and materials, especially in the preparation of polyethylene 2,5-furandicarboxylate (PEF). While the conventional synthesis of FDCA involves oxidation of 5-hydroxymethylfurfural (HMF) as a substitute, the thermal and chemical instability of HMF due to its aldehyde group poses challenges. A more favorable alternative is the utilization of 2,5-bis(hydroxymethyl)furan (BHMF), a non-aldehyde and more stable precursor. This study pioneeringly reports nitrogen-doped-carbon encapsulated cobalt (Co@NC) chainmail nanowires for the thermal and electrocatalytic oxidation of BHMF to FDCA. The Co@NC/NF achieved a 97.9 % conversion of BHMF with a 93.3 % yield of FDCA at 1.475 V vs. RHE, whereas thermal catalysis only obtained 14.9 % FDCA yield after 10 hours. Kinetic studies indicated that the large electrochemically active surface area and excellent kinetic parameters contribute its superior electrochemical performance. Mechanistic analysis revealed that the migration of inner electrons to the exterior modified the electronic properties of the carbon layer, thereby facilitating the oxidation of BHMF. Furthermore, the in-situ generation of high-valent cobalt species markedly accelerated the BHMF oxidation. This research underscores the potential of carbon-encapsulated metal chainmail catalysts in thermal and electrochemical biomass conversion.
研究领域:
化学
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材料科学
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可再生资源与环境
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xinran Wang,Xufeng Zang,Xin Wang,Wenjie Zhang,Yishan Fang,Bo Cui
The common detection methods of phoxim mostly rely on the output mode of single signal, which is easily disturbed by complex environmental media and causes errors. Herein, in order to improve the reliability of detection, we developed a dual-mode detection strategy based on nanozyme for the detection of phoxim. Firstly, manganese-nitrogen co-doped carbon nanozyme (Mn@NC) with peroxidase-like activity was synthesized by one-step pyrolysis, which was used to construct in the luminol-H 2 O 2 electrochemiluminescence (ECL) system with molecularly imprinted polymer (MIP) technology. Among them, Mn@NC can act as a co-reaction promoter to catalyze H 2 O 2 to produce large amounts of hydroxyl radicals ( • OH), thereby significantly amplifying the cathode signal of luminol and improving the stability of the signal. Benefiting from the specific selection of phoxim by MIP, this molecularly imprinted electrochemiluminescence (MIECL) mode has considerable sensitivity and selectivity, with a low limit of detection (LOD) of 0.011 ng/mL (S/N = 3). Moreover, the • OH produced by Mn@NC-catalyzed H 2 O 2 oxidized the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxidized TMB (oxTMB). Taking advantage of the fact that the simultaneous presence of acetylcholinesterase (AChE) and acetylthiocholine (ATCh) inhibited the activity of Mn@NC. A sensitive and simple colorimetric pesticide sensing platform was constructed by combining the nanozyme with the TMB-H 2 O 2 system to achieve the colorimetric detection of phoxim, with the LOD as low as 1.27 ng/mL. The dual-mode sensor was successfully applied to the determination of phoxim in agricultural products with satisfactory results, showing its great potential in the monitoring of food hazards.
研究领域:
分析化学
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食品安全
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环境科学
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
You Chen,Chunxiang Lu,Shuxia Yuan,Zhifei Liu,Xiaodan Ren,Shijie Wu
Lithium-sulfur batteries (LSBs), with their high theoretical energy density and specific capacity, are considered optimal candidates for next-generation energy storage systems. However, significant challenges remain in their cycle life and efficiency for practical applications, primarily due to the shuttle effect of lithium polysulfides (LiPSs) and the poor electrical conductivity of sulfur materials. The key to addressing these challenges lies in designing materials with excellent dispersion, good electrical conductivity, and high catalytic activity. In this work, we have designed and successfully synthesized a unique structural material consisting of in-situ grown cobalt sulfide nanoparticles embedded in zeolite imidazolate frameworks (ZIFs), which are derived from N -doped carbon wrapped around polypyrrole-derived N -doped carbon nanotubes (CoS@NC/NCNT). This design effectively mitigates the shuttle effect of lithium polysulfides (LiPSs) and enhances the conductivity of the material. As a result, batteries with CoS@NC/NCNT-modified separators achieved a high specific discharge capacity of 1518 mAh g −1 at 0.1 C. This work provides a reliable design strategy for synthesizing N -doped carbon nanotube/high-activity transition metal sulfide composite materials and opens new avenues for enhancing the modification and separation of high-performance lithium-sulfur batteries (LSBs).
研究领域:
材料科学
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能源存储技术
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PubMed
高影响因子
Small
·
2026
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IF 12.1
Xilin Wang,Ming Yue,Rongjie Xia,Hongxiao He,Yanhe Xiao,Baochang Cheng,Shuijin Lei
2D layered transition metal thiophosphites (MPS 3 ) are promising high-capacity anodes for sodium-ion batteries (SIBs) but are plagued by poor conductivity and severe volume changes. To address these challenges, we report a corn-like multi-MPS 3 heterostructure engineered via a sophisticated MOF-on-MOF templating strategy. This unique architecture, comprising a FePS 3 /ZnPS 3 heterojunction and a conformal N-doped carbon (NC) coating, establishes an interfacial field and spatial confinement synergy that facilitates rapid ion/electron transport and ensures exceptional structural integrity. The designed FePS 3 -ZnPS 3 -C@NC anode delivers remarkable sodium storage performance: a high initial discharge capacity of 1294.5 mAh g −1 at 0.1 A g −1 and long cycling stability with 87.6% capacity retention after 1200 cycles at 2 A g −1 . Such superior performance is attributed to: (i) the elastic carbon coating, which effectively buffers mechanical strain and preserves structural stability; and (ii) the heterointerfacial synergy, which enhances charge carrier mobility and reaction kinetics. Ex situ characterizations unravel a multi-mechanistic sodium storage process, accounting for the high capacity. Density functional theory (DFT) calculations confirm that the built-in electric field at the FePS 3 /ZnPS 3 interface optimizes Na + adsorption energy and interfacial charge transfer. This study provides a generalizable design paradigm for high-performance anodes through the rational integration of architectural control and interfacial engineering.
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Journal of Energy Chemistry
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2026
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IF 15.6
Yichi Guan,Lizhi Gao,Daoxiong Wu,Jie He,Hongxian Luo,Qiao Liu,Yu Zhou,Junming Luo,Ruisong Li,Zhenye Kang,Jing Li,Xinlong Tian,Shaoqing Chen,Zhengpei Miao
Iron-nitrogen-carbon (Fe-NC) materials have emerged as leading candidates among non-precious metal catalysts for the oxygen reduction reaction, offering a potential replacement for platinum-group metals in proton exchange membrane fuel cells (PEMFCs). However, the high intrinsic activity of current Fe-NC catalysts is often accompanied by rapid degradation, primarily due to the prevalence of M-N x active sites embedded within microporous carbon frameworks, which exhibit limited resistance to demetallation. Here, we report the development of mesoporous carbon-dominated Fe-NC (MC-Fe-NC) catalysts featuring atomically dispersed Fe-N 4 active sites (5.62×10 19 sites g −1 ), synthesized via a dual-coordination strategy combined with an assisted in-situ pore-forming approach. Mechanistic investigations reveal that the interconnected mesoporous architecture improves mass transport and water management at the electrode/membrane electrode assembly level, thereby mitigating carbon corrosion and structural degradation during durability testing. MC-Fe-NC demonstrates superior durability under stringent H 2 /air conditions, retaining 82% of initial current density at 0.6 V for 36 h, 92% of initial voltage at 0.2 A cm −2 for 100 h and enduring 30000 square-wave voltage cycles—surpassing the performance of most previously reported Fe-NC systems. Distribution of relaxation time analysis further supports that the mesoporous structure alleviates water flooding and carbon corrosion-related transport deterioration. Density functional theory calculations reveal that the N-enriched local coordination environment downshifts the d -band center, weakens OH-related perturbations, and reduces the driving force for metal dissolution, thereby enhancing the intrinsic anti-dissolution capability of the active sites. These results indicate that the improved durability originates from the synergistic effect of the interconnected mesoporous architecture and the N-enriched local coordination environment. This work offers a rational design pathway for stabilizing single-atom catalytic sites through the optimization of mesoporous structure and local coordination environment, advancing the practical deployment of non-precious metal catalysts in PEMFCs.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Run Cai,Jiahao Jiang,Pengfei Diao,Zihan Wei,Change Yao,Bosheng Zhou,Huijuan Zhang,Wenwen Liu,Zhong Ma
It is crucial to develop low-cost and efficient electrocatalysts to facilitate oxygen reduction reaction (ORR) and transition metals incorporated into nitrogen-doped carbon matrices (M-NC) catalysts are regarded as a potential candidate to substitute platinum-based electrocatalyst. However, there is still a great challenge in real activity and stability, compared to Pt-based electrocatalysts, for large-scale applications. An effective way to improve the ORR performance for this category of single-atom catalysts is to increase the density of active sites. In this work, therefore, the highly dispersed ZIF-67-derived Co-NC confined in carbon pores electrocatalysts are synthesized by impregnating ZIF-67 precursors into the nanopores of Ketjenblack EC-600JD (KB) resulting in the in-situ growing of small crystals in the pores followed by the high temperature pyrolysis. The as-prepared CoNC-700@C electrocatalyst exhibits excellent ORR performance in alkaline media with an onset potential of 967 mV and a half-wave potential of 892 mV (vs. RHE), which is much higher than that of the commercial Pt/C catalyst. It is inferred that the excellent ORR activity of CoNC-700@C mainly results from the increased density and also enhanced dispersion of active sites due to the confinement effect offered by the pores of KB. This study also provides a simple and effective method to increase the density of active sites for single-atom category materials.
研究领域:
材料科学
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电化学
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高影响因子
NEW CARBON MATERIALS
·
2026
·Vol. 40
·期 6
·1292-1303
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IF 6.8
Zong-da TIAN,He-feng YUAN,Zi-zai MA,Yong-feng LI,Xiao-guang WANG
Nickel nanoparticles (Ni NPs) encapsulated in carbon shells have shown promise in the electrochemical reduction of CO 2 to CO. The electronic regulation of the interface between Ni NPs and carbon shells plays a crucial role in reducing the energy barrier of the CO reaction path. We report the formation of a catalyst with hierarchical porosity (Ni NPs@NC) using a high-surface-area 3D Ni-MOF as the precursor. By correlating the pyrolysis temperature with structural changes and catalytic efficiency, structure-activity relationships were established. Because of the confined encapsulation of the Ni NPs by the N-doped carbon layer, the framework does not collapse during pyrolysis but also produces a high-density of exposed Ni-N active sites and better mass transport paths. Notably, the Ni NPs@NC-800 sample had an outstanding electrocatalytic performance for CO 2 reduction, achieving a maximum Faradaic Efficiency (FE) of 93% at −0.8 V vs RHE, and maintaining over 90% efficiency even after 48 h of continuous operation. Raman spectroscopy showed that the interface between the Ni NPs and the carbon shell play a critical role in stabilizing the critical COOH intermediate, promoting CO desorption and inhibiting the competing hydrogen evolution reaction. This work may provide insight for producing catalysts for efficient electrochemical CO 2 reduction over a wide potential range. Download: Download high-res image (53KB) Download: Download full-size image
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