INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2025
·Vol. 27
·期 1
·434
·
IF 4.9
Mingyuan Zhang,Jinru Wang,Caihan Zhu,Yuning Zhang,Dewei Li,Shuozhen Hu
Developing efficient and durable oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cell technology and sustainable energy conversion. In this study, a scalable strategy was employed to synthesize ZIF-derived nitrogen-sulfur co-doped carbon nanosheets embedded with in situ generated ZnS and Co9S8nanoparticles. The synergistic effect of heteroatom doping and metal sulfide modification effectively modulated the electronic structure, optimized charge transfer pathways, and enhanced structural stability. The optimized catalyst exhibited a half-wave potential of 0.83 V vs. RHE, close to that of commercial 20 wt% Pt/C (0.85 V), excellent 4e−ORR selectivity, and exceptional stability, with only a ~15 mV degradation after 10,000 cycles. These results demonstrate that the combination of nitrogen sulfur co-doping and in situ metal sulfide addition pro-vides an effective approach for designing highly active and durable non-precious metal catalysts for the ORR. This synthetic concept provides practical guidance for the scalable preparation of multifunctional nanomaterial-based catalysts for electrochemical energy applications.
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2011
·
IF 3.65
Yan Liang,Shaoling Song,Huiqin Yao,Naifei Hu
Poly( N -isopropylacrylamide) (PNIPAM) hydrogel films containing glucose oxidase (GOD), designated as PNIPAM-GOD, were synthesized on the surface of pyrolytic graphite (PG) electrodes through radical cross-linking polymerization method. Cyclic voltammetric (CV) response of ferrocenecarboxylic acid (Fc(COOH)) at PNIPAM-GOD film electrodes was very sensitive to the environmental temperature, sulfate concentration, and addition of methanol solvent. For example, at 25 °C, Fc(COOH) exhibited a quasi-reversible CV peak pair with large peak currents in pH 7.0 aqueous solutions containing no sulfate for the films; while at 37 °C, the CV response was greatly suppressed. By switching the film electrodes in solutions between 25 and 37 °C, the CV peak currents of Fc(COOH) cycled between a quite large value and a very small one, showing the reversible thermo-sensitive switching property between the on and off states. Similarly, the reversible SO 4 2− - and methanol-sensitive on–off behavior of the films toward the probe was also observed. This triply responsive property could be used to realize the thermo-, SO 4 2− -, and methanol-controlled electrochemical oxidation of glucose catalyzed by GOD immobilized in the films and mediated by Fc(COOH) in solution. This “smart” interface may establish a foundation for fabricating a novel type of multi-controllable biosensors based on bioelectrocatalysis.
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高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Xue Ma,Xin Dong,Baosheng Li,Qiuyue Zheng,Rui Li,Chaobo Huang,Lihua Huo,Xianfa Zhang,Xiaoli Cheng,Yingming Xu
n-Pentanol, a commonly used Volatile organic compounds (VOCs) in industry, is harmful to the environment security and human health. Thus, it is necessary to develop n-pentanol sensors. Herein, spherical (ZTO-S), cubic (ZTO-C) and pseudo-cubic (ZTO-PC) ZnSnO 3 were obtained by changing the ratio of solvent in hydrothermal/solvothermal process. By contrast, the ZTO-PC sensor had a high sensitivity of 135.2 to 100 ppm n-pentanol at 170 °C, a short response time of 0.8 s, and a low detection limit of 10 ppb. Meanwhile, the ZTO-PC sensor displayed superior reproducibility, good humidity resistance and excellent long-term stability. The outstanding sensing performance response of the ZTO-PC sensor is attribute to its high surface adsorbed oxygen content, fast electron mobility and good conductivity, providing abundant active sites and effective gas adsorption platform. In addition, the mechanism of the ZTO-PC sensor for n-pentanol was studied by XPS , GC-MS, and in-situ DRIFTS . After contact with ZnSnO 3 , n-pentanol was first oxidized to n-pentanal and then decomposed into CO 2 and H 2 O. This work well-designed three types of ZnSnO 3 through morphological engineering, providing a hopeful strategy for improving the gas sensitive performance.
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Industrial Chemistry & Materials
·
2023
·
IF 0
Yu Chen,Chang-Long Tan,Jing-Yu Li,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Photocatalytic hydrogen (H2) production coupled with selective oxidation of organic compounds into high-value-added organic intermediates has expansive prospects in the utilization and transformation of solar energy, which meets the development requirements of green chemistry. In this work, high-efficiency hole cocatalyst PdS-decorated In2S3 flower-like microspheres are fabricated for the effective visible-light-driven C–N coupling of amines to imines coupled with H2 evolution. Owing to the establishment of the internal electric field, which further boosts the transfer of photoexcited holes to PdS, PdS–In2S3 exhibits distinctly enhanced photocatalytic redox performance, which is 39.8 times higher for H2 and 14.3 times higher for N-benzylidenebenzylamine than that of the blank In2S3, along with high selectivity and stability. Furthermore, the practicability of dehydrogenation coupling of various aromatic amines to the corresponding C–N coupling products on PdS–In2S3 has been demonstrated and a plausible reaction mechanism has been proposed. This work is anticipated to stimulate further interest in establishing an innovative photoredox platform for selective organic synthesis coupled with H2 evolution in a green and sustainable way.
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Journal of Physical Chemistry C
·
2020
·
IF 4.189
Jingdong Yang,Xueyan Xu,Xufeng Zhou,Shunqiong Jiang,Wen Chen,Siqi Shi,Da Wang,Zhaoping Liu
Co3O4 nanoparticles with smaller particle size can expose more active sites to react with electrolytes, thereby exhibiting better supercapacitive performance. However, the size of Co3O4 nanoparticles is difficult to be effectively controlled in traditional carbon matrices. Herein, P, N-codoped carbon matrices with ultrahigh surface area and abundant nanocavities are used as a novel host to confine the growth of Co3O4 nanoparticles. The Co3O4/carbon composites with high redox activities of Co3O4 are successfully obtained, in which Co3O4 nanoparticles are strongly anchored in the carbon matrices, resulting in the enhancement of the composites’ capacitive performance (1310 F g–1 at 0.5 A g–1). Meanwhile, the strong anchoring effect of the carbon host on Co3O4 nanoparticles because of the rich doping elements and the confinement effect of the nanocavities ensure long-term stability (92% capacitance retention after 5000 cycles). Furthermore, the assembled asymmetric supercapacitor using this composite as the cathode material and activated carbon as the anode material delivers a high energy density of 47.18 W h kg–1 at 375 W kg–1.
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高影响因子
Science China-Materials
·
2024
·
IF 6.8
Wei Yi,Song Menglin,Li Lihua,Ma Yingjin,Lao Xinyue,Liu Yuan,Li Guogang,Hao Jianhua
Persistent luminescence nanomaterials can remain luminescence when the light source is turned off, which exhibits promise in biosensor and bioimaging fields since they have the ability to completely eradicate tissue autofluorescence. Although significant progress has been made in the persistent luminescence biosensing, there is still a dearth of long-afterglow detection platform with low limit of detection (LOD) and high sensitivity. Herein, Zn 2 GeO 4 :Mn, Cr persistently luminescent nanorods (PLNRs) with superior persistent luminescence and long afterglow time were developed. The addition of Cr 3+ manifestly improves persistent luminescence intensity and afterglow duration through creating a deep defect trap. Then the biosensors were constructed by combining the Zn 2 GeO 4 :Mn,Cr PLNRs-antibody and Fe 3 O 4 magnetic nanoparticles (MNPs)-antibody for nucleocapsid protein detection based on electrostatic attraction. The LOD value for nucleocapsid protein realizes as low as 39.82 ag/mL, which is much lower than the previously reported persistent luminescent-based biosensors. Accordingly, the low detection sensitivity is attributed to fluorescence resonance energy transfer. In addition, high specificity is also achieved. Therefore, the as-prepared Zn 2 GeO 4 :Mn,Cr persistently luminescent materials can act as the promising candidate in biosensors applications. This strategy provides effective guidance for the development of biosensing platforms with high sensitivity and specificity.
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2024
·
IF 5.8
Xian Huang,Shangshu Peng,Shengshang Lu,Xinhai Wang,Yang Wu,Linxi Dai,Bo Chen,Quan Xie,Yunjun Ruan
Considerable attention has been devoted to creating porous carbons with exceptional surface area and porosity from biomass waste for energy storage devices. Herein, we employed a straightforward high-temperature carbonization and KOH activation method to synthesize nitrogen (N) and oxygen (O) co-doped porous activated carbons derived from luffa vines (LVACs). The impact of varying KOH concentrations on the morphology, structure, and electrochemical properties of LVACs was thoroughly investigated. The optimal mass ratio of KOH to LVACs at 1:6 achieved the maximum specific surface area of 3369 m 2 g −1 . At a current density of 1 A g −1 , the LASC-6 electrode exhibits an impressive specific capacitance of 348.5 F g −1 . It also demonstrates exceptional rate performance, retaining 70.6 % of its capacitance at a current density of 20 A g −1 . The electrode possesses robust cycling stability, retaining 90 % of the initial capacitance after 5000 cycles. We assessed the practicality of LVAC-6 by constructing symmetric supercapacitors (SSCs) using KOH and [BMIM]BF 4 electrolytes. The KOH and [BMIM]BF 4 SSCs achieved specific capacitances of 86.75 and 50.31 F g −1 , respectively, at a current density of 0.25 A g −1 . Moreover, the [BMIM]BF 4 SSC exhibited an impressive energy density of 51.05 Wh kg −1 at a power density of 346.15 W kg −1 . Therefore, we propose a simple and cost-effective strategy to produce porous carbon materials with excellent electrochemical performance from discarded biomass waste, facilitating the preparation of environmentally friendly electrode materials for high-performance supercapacitors.
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高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 16
·4151-4158
·
IF 7.962
Huai Liu,Ning Ding,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Huayu Fang,Tianyuan Li,Lu Lin
Graphical No base needed : N-doped carbon-supported CoCu bimetallic catalyst with enhanced O 2 activation ability and basicity is demonstrated as an effective catalyst for the oxidative esterification of 5-hydroxymethylfurfural. The introduction of Cu significantly enhances the catalytic activity, resulting in a high furan-2,5-dimethylcarboxylate yield and an impressive formation rate, paving the way for the efficient and green synthesis of sustainable bio-based polymer monomers. The direct fabrication of furan-2,5-dimethylcarboxylate (FDMC), a promising renewable monomer, from biomass-derived 5-hydroxymethylfurfural (HMF) is a cutting-edge process. In this contribution, an elaborately designed N-doped carbon-supported CoCu bimetallic catalyst (Co x Cu y -NC; x / y= 9:1, 7:3, 4:6, which represents the designed molar ratio of Co and Cu in the catalyst), which could offer a desirable FDMC yield of 95 % under mild and base-free conditions (Co 7 Cu 3 -NC, 2 bar O 2 , 80 °C, 4 h) is described for the oxidative esterification of HMF. Notably, an FDMC formation rate of 6.1 mol FDMC mol Co −1 h −1 was achieved over Co 7 Cu 3 -NC, which represents the highest catalytic efficiency so far among Co-based catalytic systems. It has been demonstrated that Cu-doping in Co 7 Cu 3 -NC catalyst brings about more active sites (Co-N x species) with stronger molecular oxygen activation ability. The increase of surface N content of Co 7 Cu 3 -NC also improves basicity of the catalyst, which favors the hydrogen abstraction process during the HMF oxidative esterification reaction. These findings may pave an efficient and green way for the synthesis of sustainable bio-based polymer monomers.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 5
·053505
·
IF 4.386
Yanfang Song,Jinxiong Wu,Jiliang Zheng,Yiwei Sun,Andrei Ivanets,Guangming Du,Xintai Su
The doping of multiple heteroatoms can improve the electrochemical properties of carbon substrates. However, in existing studies, carbon, iron and nitrogen sources are generally mixed directly and then pyrolyzed for secondary activation. This tends to form aggregates of metal particles or metal oxides and requires the consumption of large amounts of alkali and energy. Therefore, there is an urgent need to develop an environmentally friendly technology capable of uniformly doping iron and nitrogen into carbon materials. In this work, porous Fe–N–C composites were prepared at 600 °C using potassium humate (HA-K) obtained from cotton straw by low-temperature pyrolysis as the carbon source, and urea-iron complexes formed by the pre-coordination of urea and Fe as the iron and nitrogen sources. In the absence of secondary activation, the best sample Fe-NHPC-2 had a good mesoporous structure with high specific surface area (889. 01 m2 g−1). It had a high specific capacitance of 256.8 F g−1 at a current density of 0.5 A g−1. The capacitance retention was 92.6% after 10,000 cycles at a current density of 10 A g−1. In the symmetric supercapacitor application, the energy density reached 33.16 Wh kg−1 when the power density was 600.2 W kg−1.
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高影响因子
Cell Reports Physical Science
·
2022
·
IF 7.832
Wenwen Zha,Qiushi Ruan,Lingqiao Kong,Xufeng Xi,Muhammad Ali Turgunov,Wei Zhang,Kun Chang,ZhengMing Sun
Graphitic carbon nitride is a benchmark n-type polymer photocatalyst for hydrogen evolution from water in suspension systems, though it is extremely inefficient in photoelectrochemical (PEC) systems. Minimizing the considerable discrepancy between the two systems is challenging but necessary for applications. Efficient electron collection on the catalyst surface is key to carbon nitride’s photocatalytic hydrogen evolution performance in suspension systems, but it is rarely achieved in PEC films because of the electron transfer barrier from bulk to the surface. Here, we report a hydrogel-based PEC photocathode that inherits the intrinsic advantages of suspension systems, providing a suspension-like environment for carbon nitride hydrogen evolution. This promotes electron trapping at heteroatom-induced shallow surface trap states, mitigates space charge layer, and reduces charge migration distance in hydrogel-supported heteroatoms-doped carbon nitride nanosheets, enabling efficient electron collection on the surface, leading to 10-time improvement in photocathodic performance. This study provides proof of concept for mimicking suspension in photoelectrodes that can be applied to various powder-based photoelectrochemical cells.
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高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2015
·Vol. 30
·期 5
·1098-1102
·
IF 0.399
Zhou Yong,Liu Fude,Wu Haiyan,Duan Lijie,Qu Boyang
One conjugated polymer consisting of carbazole and 3-hexylthiophene moiety, poly (N-Hexyl-2,7-di(2-(4-hexylthiophene)carbazole) (PNDC), has been synthesized by ferric chloride oxidative polymerization. The monomer N-Hexyl-2,7-di(2-(4-hexylthiophene)carbazole was synthesized and characterized by IR, 1 H-NMR, 13 C-NMR and MS. UV-vis absorption spectrum, fluorescence spectrum, photoluminescence spectrum and electrochemical properties of the polymer were investigated. Polymer PNDC shows maximum peak appearing at 394 nm in UV-vis absorption spectrum, strongest fluorescence-emission at 482 nm in fluorescence spectrum and maximum emission peak at 492 nm in photoluminescence spectrum. The band-gap ( E
g ), HOMO energy ( E
HOMO ), and LUMO energy ( E
LUMO ) of the polymer were obtained as 2.58, -5.32, and -2.74 eV, respectively.
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高影响因子
Industrial Chemistry & Materials
·
2024
·
IF 0
Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu
Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.
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