Nanoscale
·
2019
·Vol. 11
·期 41
·19506-19511
·
IF 6.97
Ying Li,Tong Liu,Wenxiu Yang,Zhijun Zhu,Yanling Zhai,Wenling Gu,Chengzhou Zhu
Non-Pt catalysts with excellent performance regarding the oxygen reduction reaction (ORR) have aroused enormous interest in recent years. Herein, we propose a dual-template method to synthesize a multiscale porous Fe–N–C (FeNC) catalyst. SiO2 and Zn are used as co-templates to produce a multiscale porous structure. Chitosan and glutaraldehyde are used as building blocks to fabricate the frameworks of the hydrogel. After lyophilization and annealing treatments, FeNC aerogel with a multiscale porous structure could be obtained. The as-prepared FeNC catalyst annealed at 900 °C (FeNC-900) exhibits a larger electrochemically active surface area and an improved ORR activity compared to FeNC annealed at other temperatures. FeNC-900 shows a superior ORR performance in comparison with that of commercial Pt/C in terms of the onset potential and half-wave potential, i.e., 0.959 and 0.837 V, which are 28 mV and 10 mV higher than those of Pt/C, respectively. Multiscale porosity is responsible for the outstanding ORR performance of FeNC-900. The electron transfer number of FeNC-900 for the ORR was calculated to be 3.95, which is comparable with that of Pt/C. In addition, the FeNC-900 catalyst possesses an excellent long-term duration and anti-poisoning capacity against methanol crossover. All these results endow the FeNC catalyst with tremendous potential for use in fuel cells.
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高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Ruotong Cui,Wenlong Xu,Feng Liu,Lei Yu,Jiming Liu,Xi Chen,Yingyun Qiao,Yuanyu Tian
The structure and reactivity of coal is the core problem of coal chemistry, and solving it at the molecular level has been an international unsolved problem. The chemical similarity-based coal chemistry group elevates the study from the macroscopic to the molecular level. However, the previous free radical mechanism lacks experimental confirmation and theoretical computational support. Here, the pyrolysis products of model compounds are first utilized to predict pyrolysis. The hydrogen-donating solvent is then used as a radical trap to confirm the reaction. Subsequently, density functional theory calculations are utilized to aid in the validation. Finally, family components are utilized to demonstrate the universality of the free radical mechanism of coal pyrolysis. This work combines radical trapping with quantum chemical calculations to analyze the radical reaction mechanism of coal pyrolysis in depth at the molecular level. This will provide a theoretical basis for coal pyrolysis and clean and efficient utilization.
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高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Ying Xue,Zhuo Wang,Jinteng Kang,Caidan Hou,Ronghui Ye,Ting Zhao,Xin Li
TiO 2 -based colossal dielectric ceramics have emerged as a prominent research focus in recent years. However, their further applications have been constrained by several key limitations, including the requirement of high sintering temperature (>1400 °C), relatively high dielectric loss (>0.05, 1 kHz), and temperature stability (<200 °C). This study reports rutile (In 0.5 Ta 0.5 ) 0.1 Ti 0.87 O 1.88 F 0.12 ceramics at 1220 °C sintering using 12 % InF 3 as the acceptor In 3+ source, which exhibits a colossal dielectric constant (1.1 × 10 5 ) and an ultra-low dielectric loss (0.0071) at 1 kHz and room temperature, even loss values below 0.04 (20 Hz - 100 kHz). Notably, the thermal stabilities (10 kHz, 100 kHz) simultaneously satisfy X9E (Δε r /ε 25 °C ≤ ±4.7 %) above 300 °C. F − not only supplies electrons to enhance the semiconductivity of grains, but also decreases the oxygen vacancy and average grain size (270 ± 12.53 nm) to improve grain boundaries resistances, which reduces dielectric loss and enhances frequency and temperature stabilities. As a result, the dielectric mechanism is mainly related to internal barrier layer capacitor (IBLC) and high grain boundary resistance. Therefore, this strategy provides a creative design for developing TiO 2 -based ceramics.
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高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Mingjie Xu,Ye Xiao,Tianli Liu,Hailong Wang,Bingbing Fan,Yanhao Dong,Chang-An Wang
Proton exchange membrane fuel cells (PEMFCs) have received extensive attention in electric vehicles and drones because of their high energy and power density. However, the performance of the PEMFCs is limited by the slow kinetic process of cathodic oxygen reduction. It is necessary to develop efficient catalysts with a low cost, high activity, and good electrochemical stability. Pt–M (M = Fe, Co, Ni, Cu, etc.) alloy catalysts are among the top candidates. The lattice of Pt shrinks when charge transfer from M to Pt occurs, which lowers the energy of the d-band of Pt. It not only balances the adsorption and desorption energies of oxygen-containing intermediates but also improves the stability of catalytic sites. In this study, we report a Pt3Co alloy catalyst supported on a N-doped carbon supports. The catalyst exhibits excellent ORR activity and outstanding durability performance as compared with the commercial JM Pt/C catalyst. The half-wave potential before and after accelerated durability testing is more positive, and the mass activity and the specific activity are much higher than the commercial Pt/C in both 0.1 M KOH and 0.1 M HClO4. Besides, the hydrogen evolution reaction performance has also been significantly improved compared to the Pt/C catalyst. This method is simple and feasible, which offers a strategy for the synthesis of high-performance electrocatalysts for PEMFCs.
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Sustainable Energy & Fuels
·
2024
·
IF 5
Yuting Wu,Keru Cao,Jun Yan,Yuheng Zhang,Biao Zhang,Yanan Wang,Yong Yang,Dacheng Zhou,Qi Wang,ChunXia Liu
Electrochemical detection techniques are unable to accurately distinguish isomers with similar structures and properties due to the poor stability and selectivity of some sensors and their susceptibility to environmental interference. Bimetallic synergistically synthesized MOF materials have various types of highly ordered pores and can be used as adsorbent materials and catalyst carriers. Therefore, a composite material was developed to prepare its derivative Cu/Bi@C using a bimetallic organic skeleton (Cu/Bi-MOF) as a precursor, inheriting the large number of active sites on the surface of the MOF and large surface area, while improving the electrochemical response signal. The morphology and structure of the synthesized Cu/Bi@C composites were tested and analyzed by XRD, SEM and other characterization methods, and the electrochemical response of the Cu/Bi@C nanocomposites was analyzed by using an electrochemical workstation. In this study, a simple and highly selective electrochemical method was developed for the simultaneous determination of catechol and catechol quinone. Differential pulse voltammetry (DPV) was used for the simultaneous detection of HQ and CC. The results showed that the Cu/Bi@C electrode was able to efficiently and highly selectively detect both isomers. The Cu/Bi@C electrode could detect HQ and CC in the range of 2–600 μM and 2–800 μM, respectively, under the detection environment of pH = 6.0. The detection limits were 0.08 μM and 0.11 μM (S/N = 3), respectively. The sensor was successfully applied to real samples and showed low detection limits, good recoveries, high selectivity, stability and reproducibility. This provides a new idea for electrochemical detection and is expected to be applied in several fields.
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高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Yuwei Wang,Xiaoyan Yuan,Zhuoying Ping,Dan Wei
One-dimensional materials are broadly applied in electromagnetic wave (EMW) absorption due to their fast electron transport paths. Herein, SiC/C nanofibers (SiC/C NFs) with rough surface and fluffy structure were prepared by electrospinning, using zinc acetylacetone as a structural modifier. The morphology and microstructure of the as-prepared fibers were changed by Zn sublimation during heat treatment process, leading to significantly improve their dielectric parameters and EMW absorption performance. The minimum reflection loss (RL, dB) of the SiC/C NFs/paraffin with a filling ratio of 15 wt% was −46.77 dB, and effective absorption bandwidth (EAB, RL < −10 dB) reached 5.84 GHz at 1.96 mm. The delightful performance was mainly attributed to the fluffy microstructure caused by the Zn sublimation, the fast electron transport paths established by the fibers, and the enhanced polarization loss brought by effective heterogeneous interfaces. Therefore, a referable strategy was put forward structural engineering for the absorber of SiC/C NFs.
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高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2024
·
IF 6.8
Yi Huang,Fengling Liu,Shuhua Ren,Yuanqing Ding,Man Chi,Weiwei Huang,Wenjing Gu,Hewen Qian,Yaxia Yuan,Shurong Hou,Xiabin Chen,Lei Ma
Idiopathic pulmonary fibrosis (IPF) is a progressive and lethal lung disease with an elusive etiology. Aberrant activation of c-Jun N-terminal kinase 1 (JNK1) has been implicated in its pathogenesis. Through a combination of structure-based drug design and structure–activity relationship (SAR) optimization, a series of pyrimidine-2,4-diamine scaffold derivatives have been developed as potent JNK1 inhibitors. Compound E1 was identified with low nanomolar JNK1 inhibitory potency (IC50 = 2.7 nM). The introduction of a dimethylamine side chain has significantly enhanced the ability of E1 to inhibit c-Jun phosphorylation, surpassing the clinical candidate CC-90001. Molecular dynamics simulations revealed a binding free energy of −50.46 kcal/mol for E1. Moreover, E1 displayed satisfactory pharmacokinetic properties, with a bioavailability of 69% in rats. Furthermore, compound E1 exerted significant antifibrotic effects in a bleomycin-induced IPF mouse model and prevented a TGF-β-induced epithelial-to-mesenchymal transition in vitro. These findings position E1 as a promising lead for further drug development targeting IPF.
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Heng Guan,Yizhuo Fan,Wei Wang,Qilin Wang,Yu Chen,Shengping Ruan
As a ternary metal oxide with a suitable band gap and double catalytic center, MnWO 4 has a broad application prospect in the fields of electrochemistry, catalysis, and gas detection. In this study, MnWO 4 @C composite was synthesized by a one-step hydrothermal method and its sensitivity property to xylene was investigated. The carbon microspheres with favorable ion adsorption ability effectively inhibit the agglomeration of the reaction ions, thus producing uniformly dispersed nanoscale MnWO 4 particles with large specific surface area, which could expose more reaction sites for the high valence W 6+ with good redox ability as well as Mn 2+ catalytic activation center with d-orbit. The MnWO 4 @C composite material possesses enhanced gas adsorption and high catalytic activity. The response of the MnWO 4 @C composite (53.4, 100 ppm) is 25 times larger than that of MnWO 4 to xylene, and the modified material shows properties of lower detection limit (2 ppm), good operating temperature (157 ℃) and significant selectivity to xylene. This work provides an effective strategy to improve the sensitive activity of MnWO 4 .
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yufeng Fu,Ao Xie,Yujing Guo,Peng Song,Jinyuan Miao,Linting Cheng,Chenxi Zhu,Weijian Han,Zhiqun Bai,Yongmei Chen,Pingyu Wan,Yang Tang
Water electrolysis powered by renewable energy is widely regarded as one of the most important methods for large-scale green hydrogen production. In this work, we have prepared a high-valence gallium-doped nickel-molybdenum nitride nanocomposite (Ga-Ni/Mo 3 N 2 @C) with abundant heterojunctions by a co-precipitation step and a subsequent high-temperature treatment step. The produced Ga-Ni/Mo 3 N 2 @C material benefits from a dual modification strategy (DMS) including the Ga doping-induced internal electronic construction and the carbon shell encapsulation-derived external corrosion inhibition. This DMS not only facilitates the modulation of the intrinsic activity of Ni and Mo constituents, but also strengthens the durability of the Ni/Mo 3 N 2 active components. In hydrogen evolution reaction (HER) test, Ga-Ni/Mo 3 N 2 @C exhibits ultra-low overpotentials of 9 mV at 10 mA cm −2 and 116 mV at 100 mA cm −2 , small Tafel slope of 41.2 mV dec −1 , high conductivity of 114.8 μS cm −1 and low charge transfer resistance of 0.729 Ω cm 2 . Moreover, the Ga-Ni/Mo 3 N 2 @C electrocatalyst exhibits an ultralow Arrhenius activation energy of 14.69 kJ mol −1 , lower than those of Ni/Mo 3 N 2 (20.78 kJ mol −1 ), commercial Raney Ni (41.40 kJ mol −1 ) and Pt/C catalyst (15.24 kJ mol −1 ). The Ga-Ni/Mo 3 N 2 @C-assembled electrolyzer exhibits a lower cell voltage of 1.80 V than the counterpart cells with commercial Raney Ni (2.05 V) cathode or Ni/Mo 3 N 2 (1.85 V) cathode at 3000 A m −2 and room temperature, showing negligible deterioration in performance. The utilization of high-valence Ga atoms doping and carbon shell protection effect not only modulates material electronic structure to accelerate reaction kinetics, but also inhibits the dissolution of active sites. It is believed that this study offers a novel strategy for the development of high-performance electrocatalysts in water electrolysis.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Qianqian Song,Yingbing Zhang,Ziyang Wu,Min Kuang,Jun Chen,Jianping Yang
The electrocatalytic urea synthesis has emerged as a promising alternative strategy to replace the current energy-intensive industrial Haber–Bosch processes which are limited by sluggish C–N coupling and low selectivity because of the unmatched reduction kinetics of CO2 and nitrogen-based precursors. Herein, a thermodynamically spontaneous early stage C–N coupling pathway of *CO2 + *NO → *NOCO2 is established through the asymmetric bridging-adsorption of CO2 enabled by hydroxycarbonate-induced CO32–-Cu2+ dual sites on the tandem electrocatalyst of copper carbonate hydroxide and iron oxide grown on carbon fibers (CuCH/α-Fe2O3–CFs). This asymmetric adsorption induces a pronounced electron-deficient state of carbon atoms in CO2 due to bidirectional electron transfer toward both the CO32– and the Cu2+ centers. Coupled with the directional migration of *NO intermediates at the interface, effectively suppress the subsequent protonation of *CO2 while promoting nucleophilic attack by *NO, thereby driving spontaneous initial C–N coupling of *CO2 and *NO and significantly lowering the energy barrier of the C–N coupling step. The results demonstrate a urea Faradaic efficiency of 78.7% and urea yield rate of 1794.6 μg h–1 mgcat–1 at an ultralow applied potential of −0.20 V vs RHE, surpassing most reported catalysts to date.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Mengyin Liao,Chao Wang,Xuanhua Zhang,Chao Luan,Wenyuan Xu,Zhongyi He
Novel Pt/Co(OH)2-NiO/C catalysts based on carbon black were successfully synthesized using the hydrazine hydrate reduction method and galvanic replacement strategies. They were subsequently tested for their activity in the electrocatalytic oxidation of methanol. It was observed that the peak current density of Pt/Co(OH)2-NiO/C (8.29 A mg-1Pt) was 22.4 times higher than that of commercial Pt/C-JM (0.37 A mg-1Pt). The electrocatalytic activities and durabilities of the synchronously synthesized Pt/Co(OH)2-NiO/C catalysts were significantly better than those of PtCo/C, PtNi/C, and PtCoNi/C-X (X = 200, 400, 600) catalysts synthesized by calcination in Ar at different temperatures. The reason is that the highly dispersed Pt helps to expose more active sites on the catalyst surface, and the addition of Co(OH)2 and NiO alters the electron density of Pt, which reduces the adsorption of intermediate CO, attenuates the toxic effect, and enables more efficient oxidation of methanol.
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高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 33
·期 1
·2005074
·
IF 27.398
Yang Li,Chongjia Lin,Zuoxu Wu,Zhongying Chen,Cheng Chi,Feng Cao,Deqing Mei,He Yan,Chi Yan Tso,Christopher Y. H. Chao,Baoling Huang
Low-cost and large-area solar–thermal absorbers with superior spectral selectivity and excellent thermal stability are vital for efficient and large-scale solar–thermal conversion applications, such as space heating, desalination, ice mitigation, photothermal catalysis, and concentrating solar power. Few state-of-the-art selective absorbers are qualified for both low- ( < 200 ° C) and high-temperature ( > 600 ° C) applications due to insufficient spectral selectivity or thermal stability over a wide temperature range. Here, a high-performance plasmonic metamaterial selective absorber is developed by facile solution-based processes via assembling an ultrathin ( ≈ 120 nm) titanium nitride (TiN) nanoparticle film on a TiN mirror. Enabled by the synergetic in-plane plasmon and out-of-plane Fabry–Pérot resonances, the all-ceramic plasmonic metamaterial simultaneously achieves high, full-spectrum solar absorption (95%), low mid-IR emission (3% at 100 ° C), and excellent stability over a temperature range of 100–727 ° C, even outperforming most vacuum-deposited absorbers at their specific operating temperatures. The competitive performance of the solution-processed absorber is accompanied by a significant cost reduction compared with vacuum-deposited absorbers. All these merits render it a cost-effective, universal solution to offering high efficiency (89–93%) for both low- and high-temperature solar–thermal applications.
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