Advanced Science
·
2025
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IF 14.1
Siqi Qiu,Hao Wan,Yuechao Yao,Xiao Xu,Zhangjian Li,Yongbiao Mu,Biaolin Peng,Hongliang Wu,Jizhao Zou,Lin Zeng
Iron-nitrogen-carbon (Fe-N-C) materials are promising non-precious metal catalysts for the oxygen reduction reaction (ORR), yet their long-term stability remains a critical challenge due to the dissolution of Fe-based active sites and corrosion of the carbon support. Here, a Fe-Zr dual-atom carbon-based catalyst (Fe,Zr-NC) via a one-step solid-state synthesis method is reported. The introduction of atomically dispersed Zr–N units adjacent to Fe–N 4 centers creates a dual-metal coordination structure that modulates the local electronic environment of Fe and weakens * OH adsorption, which is the rate-limiting step in the ORR process. Density functional theory (DFT) calculations reveal that the Fe–Zr synergy positions the catalyst near the apex of the ORR activity volcano. Extended experimental EXAFS confirms a Fe–Zr distance of ≈3.30 Å, closely matching the theoretical optimum (≈3.39 Å). As a result, Fe, Zr-NC achieves a high half-wave potential (0.891 V vs reversible hydrogen electrode (RHE)) with negligible activity loss over 5000 cyclic voltammetry cycles, outperforming commercial Pt/C. In zinc–air batteries, the catalyst delivers a peak power density of 185.7 mW cm −2 and operates stably for over 453 h. This work highlights the importance of dual-atom synergy in tuning intermediate binding energies and provides design principles for next-generation ORR electrocatalysts.
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DOI
PubMed
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Narina Wang,Chaolumen Bai,Xiaomin Ge,Dan Liu,Agula Bao,Tegshi Muschin,Yong-Sheng Bao
Transamidation of secondary amides via heterogeneous strategy has remained an unsolved problem. Here we report a novel and efficient approach for transamidation and esterification of ubiquitous N -heteroaryl amides with various amines and alcohols that exploits an engineered heterogeneous supported copper nanoparticles catalyst. This method overcomes the difficulty of heterogeneous catalysts, which can only achieve transamidation of primary amide driven by the emission of ammonia gas. A broad diversity of N -heteroaryl amides containing quinolin-2-yl, isoquinolin-1-yl, pyrazin-2-yl and pyridin-2-yl directing groups convert into corresponding α-ketoamides and α-ketoesters using needle-shape copper nanoparticles supported on γ-Al 2 O 3 as heterogeneous catalyst. This environmentally benign, catalyst recyclable and easy-to-handle catalysis methodology will have great application prospects in the pharmaceutical synthesis and biological or chemical industry.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Lulu Li,Fenyang Tian,Fengyu Wu,Longyu Qiu,Shuo Geng,Menggang Li,Zhaoyu Chen,Weiwei Yang,Yequn Liu,Yongsheng Yu
Ni 4 Mo electrocatalyst stands out as the promising candidate for hydrogen evolution/oxidation reaction (HER/HOR), yet the intensive hydrogen adsorption leads to sluggish kinetics, decreasing hydrogen catalysis efficiency. Herein, the structure of Ni 4 Mo nanoparticles anchored on wafer-biscuit-like N-SrMoO 4 nanorods (Ni 4 Mo/N-SrMoO 4 ) is developed to accelerate reaction kinetics by modulating electronic structure. The designed N-SrMoO 4 support enables strong electronic metal-support interaction with Ni 4 Mo, resulting in a downward shift of d -band center and achieving thermally neutral hydrogen adsorption. Ni 4 Mo/N-SrMoO 4 exhibits HER performance with an ultralow overpotential of 15 mV at 10 mA cm −2 , superior to Pt/C ( η 10 =18 mV). The outstanding exchange current density of 10.2 mA cm −2 for HOR is three times higher than that of Pt/C (3.5 mA cm −2 ). Ni 4 Mo/N-SrMoO 4 is further assembled in anion exchange membrane water electrolyzer (AEMWE), resulting in a current density of 100 mA cm −2 at voltage of 1.71 V and the excellent stability of 300 hours. Theoretical calculations and in-situ spectroscopy indicate that the introduction of Sr in N-SrMoO 4 effectively enhances electronic metal-support interaction, facilitates the enrichment of adsorbed hydroxyl (OH ads ) on active sites and weakens hydrogen adsorption on Ni 4 Mo, thereby accelerating reaction kinetics of hydrogen electrocatalysis.
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高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Shuaipeng Wang,Shengli Zhu,Zhenduo Cui,Zhaoyang Li,Shuilin Wu,Wence Xu,Zhonghui Gao,Yanqin Liang,Hui Jiang
The quest for a cost-effective, high-performance catalyst for hydrogen production from electrolyzed water across a broad pH range holds immense importance. B, N co-doped Mo2C was first synthesized via microwave plasma chemical vapor deposition (MPCVD) for efficient hydrogen production from electrolyzed water. The B, N-Mo2C catalyst demonstrates a requirement of 81 mV in 1.0 M KOH to achieve a current density of 10 mA cm−2. Density functional theory (DFT) calculations revealed that B, N co-doping optimizes the charge transfer between H* and Mo2C, diminishes the excessive hydrogen binding energy of Mo2C, and supports effective and stable hydrogen evolution reaction (HER) conduction in diverse settings. This doping strategy offers a systematic design approach for designing highly active noble-metal-free HER catalysts.
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Jiaxue Gao,Hua Lin,Tianwei Wang,Caicheng Song,Rongwen Lu,Shufen Zhang
Nowadays, supercapacitors as energy storage devices have gradually attracted more attention. In this paper, a tailored “staggered reaction” strategy was employed to synthesize the N/S codoped hollow porous carbon nanospheres as an electrode material for high-performance supercapacitors. This manner features the appropriate involvement of the solvent acetone in the reaction within the system, which enables the sequential reaction process to obtain the core–shell structure with different internal and external compositions. Furthermore, the core could be dissolved by soaking in a formic acid solution, thereby achieving a targeted hollow structure. In addition, in situ doping was achieved by selecting suitable precursors (m-phenylenediamine and 2,4-diaminobenzenesulfonic acid) containing N and S, and the effect of N and S content on performance was investigated in detail. The results reveal that with the increase of N and S content, the specific capacitance of carbon nanospheres first increases and then decreases. Ultimately, the maximum specific capacitances of 398 and 277 F·g–1 were obtained under the current density of 0.2 A·g–1 in a three-electrode system and a two-electrode system, respectively. After 10,000 cycles, the specific capacitance can be basically maintained at 100% with excellent cycling stability.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
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IF 24.319
Xiang-Yu Lin,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Photochemical dehydrogenation of N-heterocyclic amines to corresponding N-heteroaromatics paired with hydrogen (H 2 ) production represents a promising route for the green and sustainable organic synthesis and clean fuel generation. Herein, metal-organic frameworks (MOFs)-supported CdS nanoparticles are gingerly fabricated for the visible light-initiated acceptorless dehydrogenation of diverse N-heterocycles at ambient conditions. With further nickel cocatalysts modification via a simple photodeposition method, the optimized MIL-101 @CdS-Ni composite exhibits remarkably enhanced activities, which are 8 folds higher than that of binary MIL-101 @CdS and 2.8 times higher than that of MOF-removed CdS-Ni counterparts, along with high selectivity and good stability. Mechanism studies reveal that active nickel species plays a key role in accelerating the separation of photogenerated charge carries and the cleavage of C−H and N−H bonds in the scaffold of N-heterocycles on the catalyst surface. This work is expected to guide the rational catalysts design of MOF-based multifunctional materials for photochemical coupling of concurrent organic synthesis with H 2 production.
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高影响因子
Advanced Composites and Hybrid Materials
·
2024
·Vol. 7
·期 4
·1-13
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IF 23.2
Li Mufang,Chen Huijun,Zhao Jiale,Xia Ming,Qing Xing,Wang Wen,Liu Qiongzhen,Lu Ying,Luo Mengying,Zhu Xiufang,Wang Dong
The increased human demand for an intelligent life puts forward a great requirement for lightweight, stretchable, and comfort sensing and energy harvesting devices. Stretchable thermoelectric fiber becomes very attractive due to it can directly convert human body waste heat into electricity and enables stress, strain, and temperature sensing by designing the structure of the materials. However, the preparation of stretchable poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) fibers with enhanced performances and continuous p-n alternating structure remains a challenge. In this study, the stretchable continuous p-n alternating thermoelectric fibers were prepared by a simple and controllable microfluidic wet-spinning process, in which the single-walled carbon nanotubes (SWCNT)/PEDOT:PSS/polyurethane (PU) and polyethyleneimine (PEI) doped SWCNT/PEDOT:PSS/PU were used as p- and n-type segments, respectively. To optimize the performances, the effect of SWCNT and PEI concentration on the morphology, thermoelectric, and mechanical properties of p- and n-type fibers were analyzed. The power factor of the p- and n-type fibers were 2.67 and 3.48 µW m −1 K −2 , respectively, with a stress of 16 ~ 19 MPa and strain of 70%. Then, the strain and temperature sensors were constructed by the stretchable TE fibers and used for respiration and motion monitoring, showing excellent sensitivity and stability. All the results demonstrate the multifunctions of the stretchable TE fibers used as flexible wearable electronics.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
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IF 3.9
Gao Minjie,Yang Zongmei,Song Senchuan,Liu Xigui,Wang Fei
A series of Pd/N-doped graphene catalysts were designed for the efficient and highly selective synthesis of muscone through the hydrogenation of 3-methylcyclopentadecenone (XT). The catalysts were characterized using FT-IR, BET, XPS, XRD, Raman and SEM–EDS. All results indicated the uniform dispersion of Pd on NG. By optimizing reaction conditions, the hydrogenation of XT achieved a high yield and selectivity of muscone, producing a 99% yield at 2 MPa H 2 and 90 °C in 10 h using a 10 wt% Pd/N-doped graphene catalyst functionalized with melamine (Pd/NmG), which significantly outperformed conventional Pd/C catalysts. Graphical abstract
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高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Fangyou Meng,Jiaqi Zhu,Kaiyi Shi,Xue Wang,Junhong Zhou,Shuangzhu Jia,Yuan Yu
Theoretically, the stronger electronegativity of N compared to that of P suggests that N-doped FeP4 could reduce the adsorption energy of hydrogen, potentially enhancing the kinetics of the hydrogen evolution reaction (HER) and improving its electrochemical characteristics. Experimentally, a three-dimensional (3D) porous dodecahedron N-doped FeP4 nanoparticle array catalyst developed on carbon cloth (CC) was investigated. The synthesized N-doped FeP4/CC nanoparticle electrocatalysts demonstrated satisfactory HER performance. These electrocatalysts showed a current density (J) of 10 mA/cm–2 at an overvoltage of 87 mV in a 0.5 M H2SO4 solution, indicating that the electronically modified FeP4 (N-FeP4/CC) catalyst exhibited superior HER activity. Additionally, the overpotential for the N-doped FeP4/CC nanoparticle catalyst was 347 mV for HER in simulated seawater solution (0.5 M H2SO4 + 0.5 M NaCl), demonstrating the exceptional catalytic activity of the N-doped FeP4/CC nanoparticle catalyst. Density functional theory (DFT) calculations showed that N doping could synergistically improve the Gibbs free energy of hydrogen adsorption (ΔGH*) of FeP4 (−0.29 eV), which was lower than that of undoped FeP4 (0.41 eV). This supports the theoretical proposition that modifying the electronic structure can enhance the electrolysis hydrodynamics and catalytic performance, aligning with experimental findings. This study may provide a strategy for optimizing the electronic structure of seawater splitting.
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高影响因子
DIAMOND AND RELATED MATERIALS
·
2024
·
IF 4.3
Mei-Xia Zhao,Bo Meng,Juan-Juan Zheng,Ning Yang,Fang-Jing Liu
Lignite-derived residue with cross-linked aromatic structure and heteroatom groups is an alternative and low-cost precursor for porous carbon. Herein, N-doped hierarchically porous carbon (NDHPC) was prepared by KOH activation from lignite-derived residue using ZnO as the template and dicyandiamide as the nitrogen source. The optimal NDHPC presents hierarchically porous stacked layered structure with high specific surface area (2648.18 m 2 /g) and contains abundant O/N functional groups, making it promising candidate as the electrode material. Introducing nitrogen can provide more pseudocapacitors and meanwhile improve the wettability of the NDHPC, thus enhancing electrochemical performance. The optimal NDHPC exhibits a high specific capacitance of 336 F g −1 at the current density of 0.5 A g −1 with good rate performance. Additionally, the assembled NDHPC symmetrical supercapacitor presents outstanding cycle stability with 96.2 % capacitance retention and possesses energy density of 7.85 Wh kg −1 at power density of 250 W kg −1 . This study offers an effective and low-cost approach to fully utilize the organic matter in coal-derived residue for preparing supercapacitor electrode materials.
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高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Rong Deng,Zhilan Wang,Jing Chen,Lianqin Zhu,Yaqin Shi,Wenli Xue
Ti 3 C 2 QDs with good water solubility and photoluminescence properties was prepared by nitrogen and phosphorus doping (N,P-Ti 3 C 2 QDs). The probe has a fluorescence emission peak at 420 nm and emits bright blue fluorescence, which can distinguish and detect two antibiotics with similar structures, chlortetracycline (CTC) and tetracycline (TC). The fluorescence enhancement effect can be realized by the interaction with CTC. The linear range is 2–22 μM, and the detection limit is as low as 0.53 μM. And the change of fluorescent color from bright blue to bright purple can be observed with the naked eye. At the same time, with the addition of TC, the fluorescence of N,P-Ti 3 C 2 QDs can be quenched by static quenching effect, and the fluorescence color changes from bright blue to yellowish green. The detection range is 4.1–20.5 μM, and the detection limit is as low as 0.16 μM.Therefore, on this basis, a strategy for simultaneous detection and recognition of CTC and TC is proposed. The method has been successfully applied to the determination of CTC and TC in milk samples. This paper provides a new detection method for the identification of tetracycline antibiotics and taps the application potential of Ti 3 C 2 QDs in food detection.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Tiantian Liu,Jing Li,Xiaorui Yan,Kairui Li,Wenhua Wang,Haisheng Wei
The availability of catalytic sites for contact with reactants is a key issue to improve the performance of a catalyst, where constructing hollow structured nanomaterials has been considered as an effective strategy. Here, an N-doped carbon supported Ru catalyst with an interior cavity was synthesized by etching a MOF-derived core–shell precursor, in which metal Ru can be highly dispersed in the porous shell. This catalyst shows 98.7% conversion and >99% selectivity towards p-chloroaniline in the hydrogenation of p-chloronitrobenzene, which is better than the corresponding supported catalyst. Moreover, it also displays excellent stability with 5 cycle runs and good substrate universality for the hydrogenation of extensive substituted nitroarenes. Various characterization techniques and control experiments reveal the advantage of the unique structure to promote the mass transport and adsorption of reactant molecules on Ru sites. This work provides a novel strategy to design an efficient Ru-based catalyst for chemoselective hydrogenation.
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高影响因子
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