Small Methods
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2026
·
IF 8.7
Enmin Lv,Yilong Wang,Hongtao Yu,Hao Zhang,Xuefeng Zhang,Xinglong Dong
Developing efficient non-precious oxygen reduction reaction (ORR) catalysts is essential for advancing zinc-air batteries (ZABs). This work presents a one-step synthesis of core-shell Cr 3 C 2 @C nanoparticles (NPs) via DC arc-discharge plasma. Precise regulation of cooling dynamics achieves a switch from growth-dominated to nucleation-dominated regimes, enabling controlled preparation of nanoparticles with distinct sizes. The liquid-nitrogen-cooled Cr 3 C 2 @C ln NPs exhibit smaller size and higher surface area, leading to enhanced ORR performance. Subsequent nitrogen doping at 700 °C produces Cr 3 C 2 @C ln (N x ) catalysts with precisely tuned nitrogen content (0.65–1.24 at.%). The optimized Cr 3 C 2 @C ln (N 1.13 ) demonstrates outstanding ORR activity with a half-wave potential ( E 1/2 ) of 0.81 V and superior kinetics, surpassing commercial Pt/C. In situ optical emission spectroscopy (OES) monitors the plasma state and electron temperature, providing fundamental insights into nucleation mechanisms. Density functional theory (DFT) calculations reveal that nitrogen doping optimizes the p -band center of carbon and significantly reduces the energy barrier of the rate-determining step (RDS) (*OH desorption). When applied in both liquid and solid-state flexible zinc-air batteries (FZABs), the Cr 3 C 2 @C ln (N 1.13 )-based cathode delivers exceptional performance, achieving high power densities (230.64 and 164.83 mW·cm −2 , respectively) and remarkable cycling stability. This study offers an efficient strategy for designing high-performance transition metal carbide electrocatalysts through synergistic control of size and electronic structure.
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ACS Sensors
·
2026
·
IF 10.9
Cheng Linying,Zhong Yuee,Li Manqi,Huang Shu,Tang Jianru,Zhu Xiaohua,Li Haitao,Zhang Youyu,Liu Meiling
C-reactive protein (CRP), a key inflammatory biomarker, plays a critical role in clinical diagnostics; however, its reliable quantification demands analytical methods that surpass the limitations of conventional single-mode detection by integrating high sensitivity with built-in signal fidelity. Herein, we report a dual-mode photoelectrochemical (PEC) and colorimetric sensing platform based on bifunctional cobalt–ferrocene metal–organic framework (CoFcMOF) nanoflowers (NFs) for the ultrasensitive detection of CRP. The sensor is constructed on an In 2 O 3 -sensitized CdS heterojunction, which facilitates efficient charge separation and enhanced photocurrent response. The CoFcMOF NFs serve a dual function as both an antibody immobilization matrix and a peroxidase (POD)-mimicking signal transducer. Specific antigen–antibody recognition increases the interfacial electron-transfer resistance, leading to effective quenching of the PEC signal, while the POD-like activity of the CoFcMOF NFs catalyzes the oxidation of TMB, generating a distinct colorimetric readout. This integrated approach combines the advantages of intuitive visual screening and precise PEC quantification, addressing the inherent limitations of single-mode detection systems. The dual-mode platform enables simultaneous signal acquisition and achieves ultralow detection limits of 2.9 pg/mL (PEC) and 7.5 pg/mL (colorimetric) for CRP, which was also applied for CRP detection in serum and synovial fluid samples. This design offers significant synergistic advantages in functional integration, signal amplification, detection reliability, selectivity, and universal applicability, positioning it as a robust tool for the early diagnosis and disease monitoring in inflammatory arthritis and beyond. Beyond its analytical performance, this work introduces a versatile and robust paradigm for dual-mode biosensing and provides design principles for constructing multifunctional nanoarchitectures for next-generation sensing technologies.
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ANALYTICA CHIMICA ACTA
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2026
·
IF 6.1
Zimiao Wen,Xinhua Lian,Zihan Zhang,Haiyan Zhao,Na Li,Min Cui,Cong Zhang
Insulin-like growth factor-1 (IGF-1) is a critical biomarker linked to various human diseases, necessitating sensitive and reliable detection methods. Herein, we report a novel sandwich-type ratiometric electrochemical immunosensor with signal on–off capability for the ultrasensitive measurement of IGF-1. The sensor was constructed using gold nanoparticle-engineered carbonized covalent organic frameworks (Au@C-COFs) as the sensing platform and thionine-enriched alkynyl COFs (Thi@aCOFs) as the signal amplification probe. Au@C-COFs exhibited excellent electrocatalytic activity toward hydroquinone (HQ) oxidation, providing a stable internal reference signal, while Thi@aCOFs generated a concentration-dependent reporter signal upon specific recognition of IGF-1 via the immobilized aptamer. The ratiometric strategy effectively eliminated external interferences, significantly enhancing accuracy and reliability. Under optimal conditions, the biosensor displayed a wide linear range from 10 fM to 1 nM, a low detection limit of 0.45 fM (S/N = 3), good specificity, stability, and satisfactory reproducibility. Furthermore, the sensor performed well for measuring IGF-1 in diluted human serum, achieving satisfactory recoveries. This work presents a robust and adaptable platform toward ratiometric electrochemical biosensing, holding great promise to achieve clinical diagnosis and management treatment of IGF-1-related disorders.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2025
·Vol. 122
·期 43
·e2508077122
·
IF 9.1
Qizhu Qian,Qilong Liu,Mengxiang Wang,Jingjing Yang,Huiyi Li,Wei Bai,Wentao Wang,Changzheng Wu,Chong Xiao,Yi Xie
The emerging electrocatalytic C–N coupling reaction provides an attractive route toward green urea synthesis, but a lack of in-depth insight into the catalytic mechanism and the geometric/electronic configurations that determine the key C- and N-coupling intermediates formation hampers the exploration of efficient catalysts. Herein, we design a bimetallic oxide (Fe-Mo-O) with dual active sites of Fe and Mo for the adsorption and activation of NO2− and CO2, respectively. Constructing dual-metal catalyst leads to an upshift of the d-band center and the generation of an intermediate-spin Fe center, which not only favors the selective conversion of *CO2 into the key intermediate *CO on Mo sites, but also facilitates the adsorption and reduction of NO2− on Fe sites. Operando characterizations and theoretical calculations together elucidate that urea generation is associated with the formation of *CONH2 intermediate by coupling *CO and *NH2 on the alternating Mo and intermediate-spin Fe active sites, ultimately synergistically lowering the C–N coupling energy barrier. Specifically, the Fe-Mo-O catalyst delivers a high urea yield rate of 681.8 μg h−1 mg−1cat. and an excellent Faradaic efficiency of 60% at −0.5 V (vs. RHE). Furthermore, a C–N coupling paired with a glycerol oxidation system allows for energy-saving electrochemical coproduction of urea and formic acid. Our findings offer a feasible strategy to develop cutting-edge electrocatalysts for urea synthesis by active site design and electronic structure regulation.
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ELECTROCHIMICA ACTA
·
2011
·Vol. 56
·期 27
·10204-10209
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IF 3.65
Chang Su,Lihuan Xu,Botao Wu,Cheng Zhang
In this work, LiFePO 4 /C composites were prepared in hydrothermal system by using iron gluconate as iron source, and two feeding sequences during the preparation were comparatively studied. The morphology, crystal structure and charge–discharge performance of the prepared samples were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and galvanostatic charge–discharge testing. The results showed that the feeding sequences and iron gluconate seriously affected the microstructures and electrochemical properties of the resulting LiFePO 4 cathodes in lithium ion batteries. The spindle-shaped LiFePO 4 with hierarchical microporous structure self-assembled by nanoparticles has been successfully synthesized by synthesis route B. In addition, the cell performance of the synthesized LiFePO 4 by synthesis route B was better than that of LiFePO 4 by synthesis route A. Specially at high rates, the superior rate performance of the spindle-shaped LiFePO 4 /C microstructure (LFP/C-B) was revealed. And special reversible capacities of ∼118 and ∼95 mAh g −1 were obtained at rates of 2 C and 5 C, comparing to ∼96 and ∼68 mAh g −1 for LFP/C-A.
研究领域:
材料科学
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电化学
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储能技术
·
纳米材料
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Defence Technology
·
2026
·
IF 6.4
Yuhui Wang,Haobo Sun,Shaozhe Liu,Xiaorui Yan,Xin Zhao,Ruibin Liu,Penghao Bai,Zihui Meng,Zhibin Xu
3,6-dinitropyrazolo[4,3-c] pyrazole (DNPP) is an important fused heterocyclic energetic compound. A series of DNPP derivatives and their corresponding ionic salts with excellent properties have been reported, demonstrating significant application potential. However, the traditional synthetic route for DNPP presents inherent safety concerns due to the accumulation and isolation of hazardous diazo intermediates, which severely restrict its scalable and environmentally benign production. To address this issue, we proposed a novel synthetic strategy based on the in situ generation of diazonium salts. Starting from 3,5-dimethylpyrazole, DNPP was synthesized via a sequential process involving nitrosation, reduction, acetylation, cyclization, hydrolysis, nitration, oxidation, and decarboxylative nitration. This process increased the overall yield of the key intermediate, 3-methylpyrazolo[4,3-c] pyrazole, from 24.1% to 53.9%. The improved route avoids the accumulation of hazardous intermediates and offers advantages including operational simplicity, high safety, environmental benignity, excellent yield, and facile work-up, thereby demonstrating good scalability. Furthermore, the reaction mechanism was investigated using density functional theory (DFT) calculations. The single-crystal structure of DNPP was elucidated. Based on electrostatic potential and Hirshfeld surface analyses, correlations were established among its charge distribution, intermolecular interactions, stability, and chemical modifiability. Its detonation performance was experimentally evaluated and validated via the laser micro-detonation technique and initiation capability test. This study lays a foundation for the scale-up production and practical application of DNPP and its derivatives and also provides guidance for the synthesis and development of fused heterocyclic energetic compounds with superior performance.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zuyang Huang,Lianyang Huang,Shuohai Fang,Yunchuan Yang,Meidan Lai,Xin Zhong,Changzhong Liao,Zihao Wu,Jun Liu
Advanced oxidation processes (AOPs) based on photocatalysis and peroxymonosulfate (PMS) activation hold great promise for the remediation of organic wastewater. To overcome the limitation of narrow light utilization, sluggish PMS activation, and weak synergy between photocatalysis and PMS activation, the rational integration of transition-metal-mediated PMS activation with heterostructure engineering under light provides an efficient pathway for accelerating internal electric field construction and enhancing pollutant degradation. Herein, a C-LaFeO 3 anchored Co-doped g-C 3 N 4 (C-LFO/Co-CN) catalyst was synthesized via a multi-step in situ calcination strategy. When the mass ratio of C-LFO: Co: CN was optimized to 10:1:100, the C-LFO/Co-CN catalyst exhibited optimal photo-Fenton-like synergistic performance, achieving an initial 30-minute degradation rate 5.8 times higher than that under visible light alone. It was revealed that the Co sites directly interact with PMS to form high-valent cobalt (Co(IV) = O). Furthermore, the reconstruction of the internal electric field establishes a Z -scheme heterojunction. This configuration drives the directional migration of photogenerated electrons under illumination, promoting the direct involvement of photogenerated holes from the C-LFO valence band in the degradation of NOR. The influx of photogenerated electrons in Co-CN facilitates the reduction of Co valence states, while in C-LFO, the Fe sites further participate in the formation of a Co Fe valence state cycling system under the activation of PMS. These synergistic dual-metal redox cycles ultimately promote the highly efficient degradation of NOR in the (C-LFO/Co-CN)-PMS-Vis system. This study provides new mechanistic insights and theoretical guidance for efficient photocatalysis–PMS synergistic catalysts for wastewater treatment.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 20
·10556-10564
·
IF 11.9
Shengwen Zou,Jun Kang,Yuzheng Zhang,Mingjing Qi,Xiaojun Yan,Xiaoliang Zhang,Jianmei Huang
CsPbI3 as a newly emerging semiconductor material has displayed tremendous prospects for optoelectronic applications. However, the poor photoactive black-phase stability limits its further application. In this work, we introduce transition metal nickel ion (Ni2+) as a B-site substitute into CsPbI3 nanocrystals (NCs) to stabilize their black phase. The optimized CsPbI3 NCs film presents a record photoactive black-phase stability time of 54 hours under the conditions of 85 °C and 85% relative humidity, over 108 times that of the undoped film. Furthermore, the Ni2+-doped CsPbI3 NCs solutions maintain bright red emission after vigorous stirring with an equal volume of water for 200 hours (the undoped solution is almost completely quenched), and also show bright red emission after being stored in the air for 200 days (the undoped solution is completely quenched within 43 days). Meanwhile, the photoluminescence quantum yield increased from 31.48% for undoped CsPbI3 NCs to 87.69% for doped Ni-3.65% CsPbI3 NCs. We suggest that these outstanding stabilities and excellent optical properties can mainly be attributed to the increased defect formation energy after rational Ni doping and lattice adjustment by partial replacement of Pb2+ with small-sized Ni2+. Our work provides guidance for the synthesis of phase-stabilized CsPbI3 NCs and an insight into the effect of B-site doping in a perovskite lattice, providing a promising pathway to construct stable and efficient photoelectronic devices.
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ACS Omega
·
2023
·
IF 4.1
Shenyi Ding,Sarmad Ali,Shudong Zhang,Jun Zhao,Cui Liu,Muhammad Adnan Aslam,Xinling Yu,Min Xi,Lei Pan,Nian Li,Zhenyang Wang
Robust platforms and advanced biocompatible materials having diverse performances are in tremendous demand for cryopreservation of biocells, which are greatly limited by the crystallization, formation, and growth of ice crystals. The fickle structure and the arduous extraction process of modern attainable antifreezing proteins cause fatal cryoinjury of the cells making it challenging to develop anti-icing materials. Thus, designing Au colloids is an effective way to combat cell-damaging concerns during the ice freezing–thawing process. Herein, we propose an emerging biomimetic hybrid nanomaterial (AuNR@SiO2-CDs) prepared by combining the photoheating and rewarming controlling characteristics of carbon dots (CDs) and gold nanorods (AuNRs), respectively, via a SiO2 scaffold that has an optimal aspect ratio of ∼4.4. The performance of the material is applied in the freezing and resuscitation of Hela cells. The typical linkage between the AuNR and CDs not only retains the stable structure but also possesses the symmetric functional characteristics of affirmative cryoprotectant materials and sustained low cytotoxicity of cell viability >90%. The cell recovery rate of the Hela cell is significantly improved to ∼60%, which is propped up to >4% higher by the laser irradiation dose. The above hybrid material is paving a path toward novel bionic antifreezing proteins and is envisioned for ice recrystallization inhibition and rapid rewarming.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yuxiao Gong,Lian-Hua Xu,Xue-Ji Zhang,Serge Cosnier,Dan Shan
In energy conversion issues, to boost the hydrogen evolution reaction (HER), rational design and synthesis of earth-abundant transition metal phosphides-based materials as efficient electrocatalysts are of great significance. In this work, we report a facile, green and secure approach to synthesize the Fe 2 P/N doped carbon-based hollow nanoshuttles, denoted herein as NH 2 MIL-PA-900, with enhanced HER performances. The highly porous NH 2 MIL and phytic acid (PA) were carefully selected as the self-sacrificed template and etching agent to construct the hollow structure, respectively. Moreover, the in situ coordinated biocompatible PA with Fe 3+ can also be used as the phosphorus source for the metal phosphating during the subsequent high-temperature carbonization process at 900 °C. NH 2 MIL-PA-900 possesses a hollow shuttle-like nanostructure with highly dispersed Fe 2 P nanoparticles on the shell. When used as an electrocatalyst for HER, NH 2 MIL-PA-900 exhibits a low overpotential (157 mV at 10 mA cm −2 ) and a small Tafel slope (76 mV dec −1 ).
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 13
·4492-4499
·
IF 6.4
Xulong Lv,Xihui Shan,Yi Zhang,Yanjie Liang
Photostimulated luminescence (PSL) materials have attracted considerable attention in many important fields, varying from radiation dosimetry and biomedical imaging to security encryption and optical data storage. Nevertheless, monochromatic light illumination is usually used as the stimulus source to realize the absolute separation between the PSL signal and the excitation light. Furthermore, a dark environment is considered necessary to get rid of the interference from polychromatic ambient light. Herein, we report a glow-in-the-daylight material, YBO3:Pr3+, which can emit intense and long-lasting ultraviolet-C (UVC) persistent luminescence in a bright indoor lighting or outdoor sunlight environment after ceasing X-ray excitation. We note that although the YBO3:Pr3+ phosphor shows very weak UVC afterglow in darkness, remarkable enhancement of UVC persistent luminescence can be observed in a bright ambient light environment. The UVC persistent luminescence peaking at 274 nm can last for more than 24 h under the illumination of 900 lux white LED light, and the UVC luminescence signal is free from the interference of the ambient light. This enhancement of UVC persistent luminescence is assigned to the continuous and efficient photostimulation of polychromatic ambient light, which has been confirmed by comprehensive spectroscopic investigations. The appealing glow-in-the-daylight phenomenon from the YBO3:Pr3+ phosphor will not only lay the foundation to develop more UVC persistent phosphors suitable for working in a bright environment, it will also promote the widespread use of these storage phosphors across a broad range of applications such as microbial inactivation and optical tagging.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 4
·1-11
·
IF 5.7
Li Yangguang,Yang Qiaoran,Feng Yifan,Ye Bang-Ce
For practical analysis and simultaneous detection of arbutin (AR) and hydrochinone (HQ) in cosmetics, an electrochemical sensor has been designed based on nitrogen and sulfur co-doped Fe–Ni alloy (N,S-FeNi 3 /C) nanoparticles. The N,S-FeNi 3 /C has been prepared for the first time via hydrothermal synthesis and high-temperature carbonization. N,S-FeNi 3 /C not only improves the charge transfer to the surface, but also provides rich active sites and fast ion diffusion rates owing to the iron and nickel bimetallic materials. In addition, the d-band structure of transition metals (nickel and iron) introduced by the N and S atoms exhibits an electronic structure similar to that of noble metal catalysts, thus enhancing electrocatalytic activity and increasing conductivity. Additionally, the double doping of S and N atoms significantly increases the active sites of carbon atoms; thus, N-S-FeNi3/C exhibits excellent electrochemical catalytic activity for the oxidation of AR and HQ. Further, the N,S-FeNi 3 /C sensor is used for the simultaneous determination of HQ and AR by square-wave pulse voltammetry. Distinct oxidation peaks of HQ and AR are observed at potentials of +0.028 V and +0.352 V (vs. SCE). The electrical signal increases linearly in the HQ concentration ranges of 0.1–100 μM and 0.05–70 μM for the simultaneous determination of AR and HQ with a detection limit as low as 0.0476 and 0.0135 μM (S/N = 3), respectively. Thus, rapid and accurate detection of AR and HQ in spiked cosmetics is successfully achieved, with a recovery ranging from 96.4 to 104.2%, and the relative standard deviation is lower than 3.8–4.0%. Graphical Abstract
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危险品化学品经营许可证（带存储）