ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Haoqiang Zhang,Fuying Zhu,Tao Song,Yisong Ju,Congzhong Yang,Tianshu Zhang,Jiang Du,Liang Shi,Qiuling Yue,Hui Wei,Xiaozhi Zhao
Serotonin (5-hydroxytryptamine, 5-HT) is a crucial neurotransmitter, the abnormal levels of which are closely associated with various neuropsychiatric disorders and male reproductive dysfunctions. In this study, a sulfur-doped Fe–N–C single-atom nanozyme (S@Fe-CNx) was successfully synthesized, and its oxidase-like activity and catalytic mechanism were systematically investigated. The experimental results indicate that sulfur doping significantly enhanced Fe-CNx oxygen activation capacity and catalytic kinetics by effectively optimizing the electronic structure of the FeNx active centers. Leveraging its superior oxidase-like activity, we developed a H2O2-free colorimetric sensing method for the highly sensitive and selective detection of 5-HT. The method exhibited a good linear relationship between absorbance and 5-HT concentration in the range of 40 ng/mL to 10 μg/mL, achieving a low limit of detection of 6.0 ng/mL. The successful application of this method for detecting 5-HT in human serum samples demonstrates its great potential for practical use. Furthermore, we established a smartphone-based colorimetric detection platform that quantified 5-HT by correlating its concentration with the grayscale intensity of standard solution images captured by a smartphone. This approach provides a facile strategy for developing point-of-care testing platforms.
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高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2023
·Vol. 29
·期 6
·453-461
·
IF 7.1
Qiu Wenhao,Han Qing,Yu Xiaogang,Xiang Zhonghua
Developing nonprecious metal-nitrogen-doped carbon (M–N–C) catalysts with high activity and stability is critical to their widespread use in fuel cells; however, these catalysts still face considerable challenges. Herein, a novel iron atom-cluster strategy for the synthesis of iron-based N–C catalyst comprising Fe nanoparticles (Fe NPs) surrounded by Fe-N x sites is developed for oxygen reduction reactions in an acidic fuel cell. Iron oxide NPs were incorporated into zeolitic imidazolate framework-8 (ZIF-8)-derived carbon materials and pyrolyzed at high temperatures using NaCl as a modifier to produce Fe NPs and Fe-N x composite active sites. The half-wave potential of the optimized Fe NP /FeNC-NaCl material was substantially improved to 0.81 V. Furthermore, even after 15,000 cycles, the half-wave potential of the catalyst remained essentially unchanged. As a cathode catalyst for fuel cells, it realized a high peak power density of 436 mW/cm 2 under a practical H 2 -air atmosphere. Therefore, this study presents a new approach for designing and synthesizing electrocatalytic materials with high catalytic activity and stability.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 3
·034506
·
IF 4.386
Shuiyun Shen,Lin Li,Cehuang Fu,Guanghua Wei,Xiaojing Cheng,Jiewei Yin,Xiaohui Yan,Gang Wu,Junliang Zhang
A highly active Fe/N doped porous carbon electrocatalyst is constructed benefiting from the elaborate employment of benzimidazole (BIm) as nitrogen precursor. Compared with 2-methylimidazole (2-MIm), BIm can strongly capture Fe ions and strengthen the Fe–N bond, thus more Fe–N4 active sites form in the electrocatalyst with an enhanced catalytic activity towards oxygen reduction. The optimal sample exhibits a half-wave potential of 0.80 V vs RHE in acidic media.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Linlin Wang,Yafei Guo,Wenhui Zhao,Pengfei Wang,Zonglin Liu,Ting-Feng Yi
A unique 3D hierarchical network consisting of 0D carbon dodecahedra and 1D carbon nanotubes is successfully constructed via in-situ growth. • Phosphorus doping serves as a versatile modulator to induce 1D morphology formation and optimize the electronic density of iron active centers. • The optimized N, P co-doped Fe-N-C catalyst exhibits an outstanding half-wave potential of 0.884 V in alkaline media. • The assembled zinc-air battery achieves a remarkable operational lifespan exceeding 1300 h with superior structural integrity. Developing highly efficient and durable non-precious metal electrocatalysts for oxygen reduction reaction (ORR) remains a critical challenge for the practical application of zinc-air batteries (ZABs). Herein, we successfully synthesized a robust N, P-codoped Fe-N-C catalyst featuring a unique 0D/1D intertwined architecture through a phosphorus-induced heteroatom-modulation strategy. By utilizing FePc-encapsulated ZIF-8 as a precursor, the in-situ growth of 1D carbon nanotubes from 0D carbon dodecahedrons was achieved, constructing a 3D hierarchical conductive network. Experimental and mechanistic analyses reveal that P-doping serves as the key morphology director. It not only induces the formation of structural-stable 1D nanotubes to enhance electron transfer but also modulates the electronic density of Fe centers to elevate electro-oxidation resistance. Consequently, the optimized catalyst exhibits a superior half-wave potential (E 1/2 ) of 0.884 V (vs. RHE) in alkaline media. Remarkably, the as-assembled ZAB achieves an exceptional stability of over 1300 h, demonstrating the superior structural integrity and durability of the 0D/1D network. This research offers a strategic design for engineering high-performance and stable Fe-N-C catalysts through synergistic 0D/1D architecture construction. Phosphorus-induced modulation facilitates the in-situ growth of 1D nanotubes from 0D dodecahedrons, constructing an integrated 0D/1D hierarchical Fe-N-C structure. This structural engineering optimizes the electronic environment of Fe sites for enhanced ORR kinetics (E 1/2 = 0.884 V) and endows practical zinc-air batteries with an outstanding stability exceeding 1300 h. Download: Download high-res image (283KB) Download: Download full-size image
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Small
·
2026
·
IF 11.8
Hang Zhang,Yinuo Wu,Zhen Zhang,Ying Hou,Peizhi Liu,Ting Liao,Bingshe Xu,Yanhui Song,Haixia Zhang,Junjie Guo,Ziqi Sun
M-N-C single-atom catalysts have been demonstrated to be a promising class of non-noble-metal based catalysts, but their activity is largely constrained by the symmetrical electronic density distribution of the M-N 4 moieties. Herein, a ZIF-8 derived Fe/Fe dual-center catalyst (FeN 4 /FeO 5 @NC) is constructed by introducing a O-FeO 4 configuration adjacent to the Fe-N 4 sites to form asymmetric dumbbell-shaped FeN 4 -O-FeO 4 active sites, resulting in improved intrinsic activity of Fe─N─C catalyst. The dumbbell FeN 4 -O-FeO 4 dual-center catalyst features an electron transfer pathway of “FeN 4 → bridged O → FeO 4 ”, which breaks the symmetry of the electronic density distribution of the Fe moiety and regulates the position of the d-band center, increasing the electron transfer efficiency, reducing the desorption energy barrier of the rate-determining step, and enhancing the activation ability of O 2 molecules. The obtained FeN 4 -O-FeO 4 dual-center catalyst exhibits excellent ORR performance in a pH-universal range. The liquid-state Zn-air battery (ZAB) with this FeN 4 -O-FeO 4 dual-center catalyst delivers an outstanding open circuit voltage of 1.502 V and a peak power density of 246 mW cm −2 , superior to the Pt/C-cathode ZAB. This work represents an exploration of ways to improve the ORR performance of Fe─N─C catalysts and provides a paradigm for rationally designing low-cost, highly catalytic, and stable non-noble metal catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Feng-Di Tu,Zi-Yun Wu,Pan Guo,Li-Xiao Shen,Zi-Yu Zhang,Yun-Kun Dai,Miao Ma,Jing Liu,Bin Xu,Yun-Long Zhang,Lei Zhao,Zhen-Bo Wang
Platinum group metal (PGM)-free catalysts represented by nitrogen and iron co-doped carbon (Fe-N-C) catalysts are desirable and critical for metal-air batteries , but challenges still exist in performance and stability. Here, cerium oxides (CeO x ) are incorporated into a two-dimensional Fe-N-C catalyst (FeNC-Ce-950) via a host-guest strategy. The Ce 4+ /Ce 3+ redox system creates a large number of oxygen vacancies for rapid O 2 adsorption to accelerate the kinetics of oxygen reduction reaction (ORR). Consequently, the as-synthesized FeNC-Ce-950 catalyst exhibits a half-wave potential ( E 1/2 ) of 0.921 V and negligible decay (<2 mV for Δ E 1/2 ) after 5,000 accelerated durability cycles, significantly outperforming most of ORR catalysts reported in recent years and precious metal counterparts. When applied in a zinc-air battery, it demonstrates a peak power density of 175 mW cm −2 and a specific capacity of 757 mAh g Zn −1 . This study also provides a reference for the exploration of Fe-N-C catalysts decorated with variable valence metal oxides .
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xinfa Cai,Fei Ma,Jun Jiang,Xianglong Yang,Zhaowei Zhang,Zelang Jian,Meijuan Liang,Peiwu Li,Li Yu
Sensitive, on-site and multiple detection of mycotoxins is a vital early-warning tool to minimize food losses and protect human health and the environment. Although paper-based lateral flow immunoassay (LFIA) has been extensively applied in mycotoxins monitoring, low-cost, portable, ultrasensitive and quantitative detection is still a formidable challenge. Herein, a series of Fe-N-C single-atom nanozymes (SAzymes) were synthesized and systematic characterized. The optimal Fe-N-C SAzyme with highly efficient catalytic performance was successfully used as both label and catalyst in lateral flow immunoassays for mycotoxin detection. By taking advantage of the catalytic amplified system, the qualitative and quantitative detection can be easily and flexibly done via observing the test lines by naked eyes or a smartphone, with the limit of detections (LODs) of 2.8 and 13.9 pg mL −1 for AFB 1 and FB 1 , which were respectively over 700- and 71,000-fold lower than the maximum limit set by the European Union. Besides, underlying catalytic mechanisms and the active sites of the Fe-N-C SAzyme are also investigated by DFT simulation. This work not only provides a promising detection strategy for the application of advanced SAzymes but also offers experimental and theoretical guidelines to understand the active centers of Fe-N-C SAzymes and the catalytic process.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·060547
·
IF 4.386
Ruixiang Wang,Yanyang Wang,Zheqin Chen,XiaoCong Zhong,Yongmin Xie,Xiaobo Ji,Jiaming Liu,Shubiao Xia,Zhifeng Xu
Transition metal/nitrogen carbon composite (M/NC) is a highly active oxygen reduction reaction (ORR) electrocatalyst, widely used in fuel cells and zinc-air batteries. Herein, a uniform and regular PVP-assisted iron-doped nano dodecahedron (ZP0.1F/NC) is prepared by a simple and efficient one-step in-solution reaction, followed by controlled in situ pyrolysis. The synthesized electrocatalyst showed excellent electrocatalytic ORR activity in an alkaline medium. Compared with standard 20% Pt/C electrocatalyst, ZP0.1F/NC exhibited onset potential (Eonset) (0.974 V vs 0.967 V), half-wave potential (E1/2) (0.861 V vs 0.857 V) and the limiting current density (jd) was 6.373 mA cm−2 vs 5.401 mA cm−2, also better than the Fe doped ZIF-8 nitrogen composite (ZF/NC), PVP auxiliary ZIF-8 (ZP0.1/NC) and pure ZIF-8 nitrogen composite (Z/NC) synthesized by the same procedure. In addition, the zinc-air battery assembled with ZP0.1F/NC also exhibits outstanding discharge capacity, with a specific capacity and energy density of 793.3 mAh g−1 and 974.9 Wh kgZn−1, respectively, much higher than that of commercial 20% Pt/C-based zinc-air battery (719.8 mAh g−1, 842.6 Wh kgZn−1), indicating its great potential in practical energy conversion and storage.
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Nanomaterials
·
2023
·Vol. 13
·期 18
·2496
·
IF 5.3
Mengmeng Pan,Ming Wang,Linjiao Yang,Yongli Song,Ming Jiang,Xu Yu,Li Xu
Alkaline phosphatase (ALP) is a phosphomonoester hydrolase and serves as a biomarker in various diseases. However, current detection methods for ALP rely on bulky instruments, extended time, and complex operations, which are particularly challenging in resource-limited regions. Herein, we synthesized a MOF-derived Fe-N-C nanozyme to create biosensors for the coulometric and visual detection of ALP. Specifically, we found the Fe-N-C nanozyme can efficiently oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to generate blue-colored tetramethyl benzidine (TMBox) without the need for H2O2. To construct the biosensor, we incorporated the ALP enzymatic catalytic reaction to inhibit the oxidation of TMB by Fe-N-C oxidase nanozyme. This biosensor showed rapid and highly sensitive detection of ALP in both buffer and clinical samples. The limit of detection (LOD) of our approach could be achieved at 3.38 U L−1, and the linear range was from 5 to 60 U L−1. Moreover, we also developed a visual detection for ALP by using a smartphone-based assay and facilitated practical and accessible point-and-care testing (POCT) in resource-limited areas. The visual detection method also achieved a similar LOD of 2.12 U L−1and a linear range of 5–60 U L−1. Our approach presents potential applications for other biomarker detections by using ALP-based ELISA methods.Keywords:metal-organic framework;nanozyme;oxidase-like enzyme;alkaline phosphatase;visual detection
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Sustainable Energy & Fuels
·
2019
·Vol. 3
·期 12
·3455-3461
·
IF 4.912
Bomin Feng,Xiuju Wu,Yanli Niu,Wei Li,Yunxi Yao,Weihua Hu,Chang Ming Li
Fe/N–C catalysts show great potential for the oxygen reduction reaction (ORR) but their catalytic activity should be further improved for practical application. Here, we report a high performance Fe/N–C hollow sphere with excellent ORR activity in both alkaline and acidic solutions. It is synthesized via pyrolysis of a melamine/Fe-incorporated polydopamine nanosphere precursor at 800 °C in an argon atmosphere. The N-rich melamine in the precursor affords abundant N dopants to form dense Fe–Nx active sites and also facilitates the formation of micropores in the catalyst via the gasification effect, together improving the ORR activity. The as-reported Fe/N–C catalyst outperforms the Pt/C catalyst in basic media (45 mV more positive half wave potential), approaches the Pt/C catalyst in acidic media (55 mV lower half wave potential), and exhibits impressive performance in Zn–air primary batteries.
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Small
·
2019
·Vol. 16
·期 6
·1906057
·
IF 10.856
Xueping Sun,Peng Wei,Songqi Gu,Jinxu Zhang,Zheng Jiang,Jing Wan,Zhaoyang Chen,Li Huang,Yue Xu,Chun Fang,Qing Li,Jiantao Han,Yunhui Huang
Highly active and durable bifunctional oxygen electrocatalysts are of pivotal importance for clean and renewable energy conversion devices, but the lack of earth-abundant electrocatalysts to improve the intrinsic sluggish kinetic process of oxygen reduction/evolution reactions (ORR/OER) is still a challenge. Fe-N-C catalysts with abundant natural merits are considered as promising alternatives to noble-based catalysts, yet further improvements are urgently needed because of their poor stability and unclear catalytic mechanism. Here, an atomic-level Fe-N-C electrocatalyst coupled with low crystalline Fe 3 C-Fe nanocomposite in 3D carbon matrix (Fe-SAs/Fe 3 C-Fe@NC) is fabricated by a facile and scalable method. Versus atomically FeN x species and crystallized Fe 3 C-Fe nanoparticles, Fe-SAs/Fe 3 C-Fe@NC catalyst, abundant in vertical branched carbon nanotubes decorated on intertwined carbon nanofibers, exhibits high electrocatalytic activities and excellent stabilities both in ORR ( E 1/2 , 0.927 V) and OER ( E J=10 , 1.57 V). This performance benefits from the strong synergistic effects of multicomponents and the unique structural advantages. In-depth X-ray absorption fine structure analysis and density functional theory calculation further demonstrate that more extra charges derived from modified Fe clusters decisively promote the ORR/OER performance for atomically FeN 4 configurations by enhanced oxygen adsorption energy. These insightful findings inspire new perspectives for the rational design and synthesis of economical–practical bifunctional oxygen electrocatalysts.
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ACS Catalysis
·
2014
·
IF 7.572
Mei-Qing Wang,Wei-Hua Yang,Hong-Hui Wang,Chi Chen,Zhi-You Zhou,Shi-Gang Sun
Aimed at developing a highly active and stable non-precious metal catalyst (NPMC) for oxygen reduction reaction (ORR) in acidic proton-exchange membrane fuel cells (PEMFCs), a novel NPMC was prepared by pyrolyzing a composite of carbon-supported Fe-doped graphitic carbon nitride (Fe–g-C3N4@C) above 700 °C. In this paper, the influence of the pyrolysis temperature and Fe content on ORR performance was investigated. Rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) studies reveal that, with a half-wave potential of 0.75 V [versus reversible hydrogen electrode (RHE)] and a H2O2 yield of 2.6% at 0.4 V, the as-synthesized catalyst heat-treated at 750 °C with a Fe salt/dicyandiamide (DCD) mass ratio of 10% displays the optimal ORR activity and selectivity. Furthermore, the pyrolyzed Fe–N–C composite exhibits superior durability in comparison to that of commercial 20 wt % Pt/C in acidic medium, making it a good candidate for an ORR electrocatalyst in PEMFCs.
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