查找使用阿拉丁产品的科研文献

Synergistic Ag single atoms and nanoclusters on defect-engineered In2S3 for enhanced H2O2 production and in-situ pollutant oxidation

Lingzheng Feng,Wei Han,Xiaojun Guo,Jianzhang Zhu,Jiaqi Shen,Xingguo Xiao,Hudong Yan,Fei Zha,Haifeng Tian,Xiaohua Tang

Nitrogen doping introduces sulfur vacancies and lattice distortion into In 2 S 3 , which enhances charge separation and provides anchoring sites for Ag species. • Achieves a high H 2 O 2 production rate of 965 μmol g −1 ·h −1 via the 2e − ORR pathway. • DFT reveals Ag single atoms optimize *OOH adsorption; clusters boost electron redistribution. • Exhibits efficient degradation of perphenazine (95% removal within 30 min). • Operates effectively in pure water without sacrificial agents and shows excellent stability. To address the rapid recombination of photogenerated charge carriers in indium sulfide (In 2 S 3 ) and meet the growing demand for efficient photocatalytic hydrogen peroxide (H 2 O 2 ) production systems, this study proposes a rational design. Leveraging active nitrogen species generated from urea decomposition during hydrothermal treatment, we successfully doped the In 2 S 3 lattice to construct a nitrogen-modified indium sulfide (N-In 2 S 3 ) substrate, and subsequently co-anchored silver single atoms and clusters (Ag SA+C /N-In 2 S 3 ) onto it for efficient photocatalytic H 2 O 2 production and pollutant degradation. Nitrogen (N) doping induced sulfur vacancies and lattice distortion, enhancing charge separation and surface reactivity. Ag species were atomically dispersed and firmly anchored onto the N-In 2 S 3 support, serving as efficient electron sinks and active sites. The optimized Ag SA+C /N-In 2 S 3 achieved a remarkable H 2 O 2 production rate of 965 μmol g −1  h −1 in pure water via a predominant two-electron oxygen reduction reaction (2e − ORR) pathway, significantly outperforming pristine In 2 S 3 and N-In 2 S 3 . Combined with experimental characterization and DFT calculations revealed that Ag single atoms optimized the adsorption of the *OOH intermediate and reduced the reaction free energy barrier, while Ag clusters facilitated electron redistribution and enhanced oxygen activation. It also demonstrated superior photocatalytic degradation efficiency for organic pollutant like perphenazine (95% removal in 30 min). This study highlights the synergistic effect of bulk doping and surface atomic-level engineering in developing high-performance photocatalysts for sustainable chemical synthesis and environmental remediation. Download: Download high-res image (140KB) Download: Download full-size image

Analyte-Specific “Signal-On” Uranyl Sensitive Sensing Based on Temperature-Programmed Nanozyme Activity of CoOx

Bu Zhijian,Wang Linjie,Yao Yuxuan,Chen Xinyu,Tang Zheng,Du Dan,Wu Shengtao,Lin Yuehe,Liang Hao,Niu Xiangheng

As alternatives to bioenzymes, nanozymes find promising applications in biochemical sensing thanks to their recognized superiorities, but their lack of specific interactions with targets of interest seriously hinders the exploration of selective analytical strategies when no external receptors are employed. Additionally, most nanozymes exhibit poor catalytic efficiency, much lower than their natural counterparts, thus restricting the sensitivity of detection. Different from the explored “turn-off” analytical principle relying on the coordination of the target with a nanozyme catalytic product, here we proposed an analyte-unique “signal-on” strategy based on the direct target–nanozyme interaction for the sensitive sensing of uranyl via temperature-programming the peroxidase (POD)-mimetic activity of CoO x . As wet-chemical temperature increased, the oxygen vacancy (O V ) content on CoO x surfaces exhibited a volcano-type trend, and its catalytic efficiency correlated with the former positively. UO 2 2+ was found to stimulate the POD-like activity of CoO x via increasing O V , exhibiting excellent specificity against other common species. Leveraging the unique CoO x –UO 2 2+ interaction and the temperature-programmed activity of CoO x , we validated a “light-up” colorimetric approach for UO 2 2+ selective determination, achieving a wide detection range (0.01–2 μM) and a low limit (5 nM). A deployable device based on intelligent reading was further fabricated to enable on-site monitoring of the analyte. Our work provides a “signal-on” nanozyme sensing strategy for the quantification of UO 2 2+ , featuring specific response, catalytic signal amplification, and free from bioreceptors. Also, it proves a facile route to achieve dual modulation of enzyme-mimetic activity and analyte response for broader applications.

Atomic-to-Nanoscale Engineering of Piezocatalytic Heterojunctions for Ultrasound-Triggered Osteomyelitis Therapy

Lijing Chen,Chaofeng Wang,Shuilin Wu,Congyang Mao,Yuan Li,Cuihong Chen,Talante Juma,Yongping Cao,Yu Wang,Xiangmei Liu

Osteomyelitis, primarily caused by methicillin-resistant Staphylococcus aureus (MRSA), poses critical clinical challenges, including drug-resistant infections and insufficient bone regeneration. Herein, we propose a mechano-electro-chemical energy conversion paradigm based on an atomic-to-nanoscale synergistic strategy, realized by constructing a heterojunction between sulfur-doped zinc oxide and bismuth ferrite (S-ZnO/BiFeO 3 ). At the atomic level, sulfur doping induces lattice distortion and oxygen vacancies, narrowing the bandgap of ZnO. At the nanoscale level, sulfur doping modulates crystal growth, transforming ZnO nanoblocks into thinner nanosheets that establish intimate interfacial coupling with BiFeO 3 . This dual-scale synergy amplifies the piezoelectric coefficient (d 33 ) tenfold, significantly enhancing the ultrasound (US)-responsive piezocatalytic output. Under US, the enhanced piezocatalytic field facilitates directional charge migration and continuous reactive oxygen species (ROS) generation, achieving a 99.45% antibacterial rate against MRSA while effectively inhibiting biofilm growth. Transcriptomic profiling reveals that this energy conversion process eliminates MRSA via a multi-target collapse of membrane defense, ion homeostasis, and energy metabolism. Concurrently, S-ZnO/BiFeO 3 promotes osteogenic differentiation through US-triggered microcurrents and Zn 2+ release. In vivo results validated robust bactericidal potency, osseointegrative kinetics, and excellent biocompatibility. This study establishes a mechano-electro-chemical energy conversion paradigm via atomic-to-nanoscale engineering, offering a high-performance platform for precise piezocatalytic therapy.

High 1 T-phase molybdenum disulfide induced by L-cysteine as cocatalyst for Fenton-like reaction to enhance organic pollutant degradation

Bin Wen,Fan Chen,Yi Ran,Dongyun Que,Zhihao Zhang,Youwei Zeng,Yuyuan Yao

Molybdenum disulfide (MoS₂) is a promising inorganic co-catalyst for Fenton processes due to its structural durability and avoidance of secondary organic pollution. However, the conventional 2H-phase MoS₂ suffers from intrinsically low conductivity, severely limiting Fe 3+ reduction in the Fenton reaction. Herein, L-cysteine served as a multifunctional precursor during the preparation of MoS₂, promoting a slow-release sulfur supply, carbon‑nitrogen co-doping, and the prevention of restacking. The carbon and nitrogen co-doped molybdenum disulfide (CN-MoS 2 ) architecture was fabricated via a single-step hydrothermal reaction mediated by sodium molybdate, thiourea, and L-cysteine. Remarkably, benefiting from the introduction of L-cysteine, the resulting CN-MoS 2 exhibited a high 1 T-phase content (68%), abundant sulfur vacancies, and a substantially reduced particle size. CN-MoS 2 accomplished near-complete elimination of carbamazepine (CBZ) within merely 3 min, yielding a prominent apparent rate constant of 0.7111 min −1 , which is a 19-fold kinetic acceleration over thiourea-derived MoS 2 . CN-MoS₂ also exhibited high TOC removal, broad-spectrum degradation, and robust CBZ removal under various water conditions. Additionally, electrochemical analyses further verified that CN-MoS₂ reduced charge-transfer resistance and enriched electron density, thereby facilitating rapid electron shuttling to Fe 3+ . Concurrently, quenching experiments and electron paramagnetic resonance (EPR) diagnostics unambiguously validated SO 4 •- , 1 O 2 and O 2 •- as the driving reactive forces. Moreover, a continuous-flow device incorporating a CN-MoS 2 -based membrane exhibited outstanding performance in wastewater purification. This work offers a new strategy for designing high-activity co-catalysts for advanced oxidation processes.

An in-situ strategy for tuning tensile strain to enhance hydrogen electrocatalysis on nickel-based catalysts

Lijie Zhu,Zhixin Li,Guoju Huang,Zhibing Chen,Wanli Liang,Fangyan Xie,Jian Chen,Nan Wang,Yanshuo Jin,Hui Meng

New setup monitors catalytic activity in-situ under tensile stress on metal foils. • Tensile stress shifts Ni d-band center up, lowering water dissociation barrier, boosting HER. • Heterostructure enables simple tensile strain tuning in Ni to enhance catalysis. Nickel is a widely used, non-precious metal electrocatalyst in the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR). Herein, we developed a unique in-situ setup to investigate and monitor the impact of strain on the electrocatalytic properties of nickel metal by examining the HER activity of a macroscopically strained nickel sheet. The application of strain effectively optimizes the electronic structure of Ni, facilitating the accelerated dissociation of water and, consequently, enhancing the catalytic reaction. Furthermore, we synthesized Ni/Ni 0.2 Mo 0.8 N catalysts with heterostructures and induced microscopic stress on the crystal plane of Ni through these heterojunctions. The resulting Ni/Ni 0.2 Mo 0.8 N exhibited remarkable HER and HOR activity in alkaline solutions. A series of characterizations confirmed the presence of strain, and the activity of Ni was found to increase with the degree of strain. These findings introduce a novel approach for optimizing Ni-based materials in hydrogen catalysis and beyond.

Chemical Bath Solution In-Addition Enabled Grain Boundary and Heterojunction Interface Defects Mitigation Achieving 12.1% Efficiency CZTS Solar Cell

Xinyu Li,Yuqin Zhong,Hongkun Liu,Chengfeng Ma,Chunxu Xiang,Yize Li,Sifan Zhou,Na Zhao,Weibo Yan,Shaoying Wang,Hao Xin

The performance of wide bandgap Cu 2 ZnSnS 4 (CZTS) thin film solar cells is limited by serious recombination due to high concentration of defects and “cliff-like” conduction band offset (CBO) at the heterojunction. The state-of-the-art strategies tackling these issues are post heat treatment and alternative buffer layer. Here, we address these issues by adding InCl 3 to the chemical bath deposition solution (CBD-In-addition) for CdS buffer layer. At early CBD stage, In 3+ sufficiently substitute Zn 2+ near CZTS absorber surface and along the grain boundaries (GBs), enabled by smaller size than Cd 2+ and no complexation with NH 3 , resulting in highly conductive GBs with beneficial upward band bending. Further, the incorporation of In 3+ into CdS ((Cd,In)S) improved buffer layer n-type conductivity, alleviated heterojunction lattice mismatch and enlarged buffer layer bandgap, resulting in a coherent CZTS/(Cd,In)S interface, a “spike-like” CBO, and a more transparent buffer layer. These effects lead to 12.14% efficiency CZTS solar cell, improved by 31% compared to reference device (9.29%). This is the highest efficiency sulfide CZTS solar cell with chemical bath deposited buffer layer without post heat-treatment. The simple and synergetic defects mitigation strategy is expected to advance other wide bandgap chalcogenide thin film solar cells.

CuS-Bridged MXene-Based Photoresponsive Phase Change Materials Enabling Thermoelectric Cogeneration and Microwave Absorption

Feng Yuhao,Zhao Jindi,Chen Keke,Li Yang,Liu Jiao,Yu Huitao,Qin Mulin,Jia Kaihang,Han Haiwei,Shen Zhenghui,Ma Mingliang,Chen Xiao

Designing multifunctional materials integrating efficient photoresponsive thermoelectric cogeneration with microwave absorption remains challenging for clean solar energy utilization and electromagnetic interference mitigation. Herein, this study proposes an innovative design strategy combining interfacial bridging engineering and physical encapsulation to construct advanced multifunctional composite phase change materials (PCMs). A nanoparticle-bridged 3D interpenetrating phonon network is constructed via in-situ growth of CuS nanoparticles on layered MXene, creating abundant interfacial sites for polyethylene glycol (PEG) adsorption and efficient electron transport channels for electromagnetic loss. The resulting PEG-MXene@CuS composite PCMs achieve an exceptional photothermal conversion efficiency of 94.5% (100 mW cm −2 ), enabled by broadband absorption of MXene nanosheets and plasmonic effect of CuS nanoparticles. In photoresponsive thermoelectric cogeneration system, PEG-MXene@CuS serves as a heat source to drive thermoelectric module through the Seebeck effect, yielding a stable power output of 21.7 W m −2 (100 mW cm −2 ), with PEG effectively buffering thermal fluctuations. Moreover, MXene@CuS heterointerface and 3D conductive network endow PEG-MXene@CuS with superior microwave absorption, a minimum reflection loss of − 55.5 dB and an effective bandwidth of 5.27 GHz. This design concept provides important insights into designing next‑generation multifunctional PCMs with promising applications in intelligent thermal management, thermoelectric cogeneration, and electromagnetic protection.

On-Site Periodontitis Diagnosis via Room-Temperature Oral Exhalation H2S Sensor Based on Yb-Doped Bi2S3 Nanoribbon

Guo Ping,Wang Kai,An Xuyang,Ren Xuanyu,He Xinxin,Hu Yinhua,Zhou Lijie,Cai Guohua,Wang Lifeng,Liu Tiezhu,Ge Wenyu,Zhang Jia

A novel Yb-doped Bi 2 S 3 H 2 S sensor was fabricated for periodontitis exhalation diagnosis, which enables room temperature detection with high response (3.31/100 ppb) and superior selectivity. Mechanism analysis combined with density functional theory calculations confirms that Yb doping-induced lattice distortion in Bi 2 S 3 enhances O 2- formation and H 2 S adsorption. The sensor quantifies H 2 S produced by Porphyromonas gingivalis to confirm the association among pathogens, H 2 S and periodontitis, and is integrated into a portable analyzer for rapid, real‑time diagnosis and severity assessment of periodontitis clinically.

Interface Engineering Triggered Electron Transfer Channels and Enhanced p–p Orbital Coupling: Boosting CO2 Electroreduction to Formate Over Heterostructured CuS@SnO2

Jiaqi Li,Hainan Wu,Tinghui An,Yuhao Wang,Dong Xiang,Nan Wang,Kedi Cai

Tin dioxide (SnO 2 ) has been demonstrated to convert CO 2 to formate in an electrocatalytic CO 2 reduction reaction (eCO 2 RR). However, suboptimal CO 2 activation and insufficient electrical conductivity pose formidable challenges to achieving desirable eCO 2 RR activity. Herein, a heterostructured CuS@SnO 2 catalyst was designed to realize efficient formate production in eCO 2 RR, which delivers a Faraday efficiency (FE) of 94.9% and partial current density of 243.5 mA cm −2 at −1.1 V versus RHE in alkaline conditions, coupled with excellent electrochemical stability. Systematic investigations reveal that CuS acts as an electron reservoir, and the directional electron transfer channels induce interfacial electron deficiency in SnO 2 , stabilizing Sn active sites during long-term eCO 2 RR operation. Furthermore, it confers dual effects for promoting formate conversion at the molecular level, which integrates optimized interface electronic structure and enhanced p–p orbital coupling between the key * OCHO intermediate and SnO 2 interface, rendering the enhanced * OCHO adsorption, decreased CO 2 hydrogenation energy barrier, and improved intrinsic formate activity. Beyond catalytic performance, CuS@SnO 2 was further utilized in a Li-CO 2 battery to enable integrated CO 2 conversion and energy storage functionality. This study provides a strategy to effectively regulate the formate selectivity of eCO 2 RR by heterointerface engineering, and meanwhile bridges rational catalyst design with practical CO 2 conversion technologies.

In-situ reconstruction of hydrophobic environment in SnS@SBA-15 induced efficient adsorption and storage of iodine

Qiang Xian,Weijie Fan,Yulin Gu,Zishan Zhang,Jiaqi Liu,Hui Xian,Li Chen,Hui Dan,Yi Ding

New SnS@SBA-15 was developed for the efficient adsorption and storage of iodine. • The iodine adsorption capacity was up to 2062 mg/g. • The iodine adsorption mechanism was chemical adsorption (SnS + I 2 → SnI 4 + S). • The retention rate of adsorption product SnI 4 was up to 76.5% after storage for 90 d. • Stable iodine storage was due to the in-situ reconstructed hydrophobic environment. Tin-based materials are expected to be excellent iodine adsorbent, but the stability of the adsorption product (SnI 4 ) poses challenge. Herein, a novel strategy based on the in-situ reconstruction of hydrophobic environment was presented for efficient iodine adsorption and storage. Stannous sulfide@mesoporous silica (SnS@SBA-15) was developed and employed for the adsorption of I 2 gas. The optimal material, SnS@SBA-15–50wt%, exhibited an excellent iodine uptake of 2062 mg/g. The adsorption was attributed to a chemical reaction (SnS + 2I 2 = SnI 4 + S). Notably, the retention rate of SnI 4 was as high as 76.5% after storage in air for 90 days due to the in-situ reconstructed hydrophobic environment. The obtained SnS@SBA-15 exhibited efficient iodine adsorption and excellent storage ability. This work presents a novel strategy to design iodine adsorbents, aimed at addressing the storage challenges of iodine adsorption products susceptible to hydrolysis. Download: Download high-res image (214KB) Download: Download full-size image

Preparation of Oxygen-Doped Amorphous MoS2 and Its Electrocatalytic Performance for Nitrogen Reduction to Ammonia

The electrocatalytic nitrogen reduction reaction (NRR) is a key approach for synthesizing green ammonia under mild conditions. However, the high bond energy of the N≡N triple bond makes N2difficult to activate, limiting the Faradaic efficiency. MoS2offers advantages such as low cost and abundant reserves as a non-precious-metal NRR electrocatalyst. Nevertheless, pure MoS2suffers from insufficient conductivity and a limited number of active sites, resulting in suboptimal catalytic performance. Herein, we develop a solvent-regulated one-step hydrothermal strategy using ethylene glycol as the sole reaction medium to fabricate an oxygen-substituted amorphous MoS2(O-MoS2) electrocatalyst. XRD, SEM, and HRTEM characterization revealed that, as the ethylene glycol ratio increased, the product gradually transformed from a layered crystalline structure to a completely amorphous structure. XPS confirmed that oxygen atoms were uniformly incorporated into the MoS2lattice via substitution doping. Electrochemical testing showed that O-MoS2achieved an ammonia yield of 97.16 μg h−1mg−1and a Faradaic efficiency of 46.44% in a 0.1 M Na2SO4electrolyte at −0.70 V vs. RHE, significantly outperforming undoped MoS2and semi-doped S-MoS2. DFT calculations indicate that O doping reduces the N2adsorption energy, thereby synergistically promoting N2adsorption and activation. This dual-modification strategy provides a facile and universal guidance for electronic structure regulation of MoS2-based catalysts and sheds new light on the design of high-efficiency ambient nitrogen fixation electrocatalysts toward practical green ammonia synthesis.

NiFe-LDH/ZnCdS bimetallic hydroxide heterostructures for efficient multi-electron CO2 reduction

Jie Liu,Kaiyu Li,Shizhen Gao,Guohua Wu,Jing Fan

Efficient photocatalytic CO 2 reduction is limited by rapid carrier recombination and sluggish interfacial kinetics. Here, NiFe-LDH/ZnCdS (ZCS) heterostructures were fabricated by hydrothermal synthesis followed by electrostatic self-assembly. Mott–Schottky analysis, XPS, photoelectrochemical measurements, and density functional theory calculations collectively reveal staggered band alignment and interfacial charge redistribution, supporting a type-II charge-transfer pathway with improved carrier separation. The optimized 15NiFe-LDH/ZCS produced CO, CH 4 , C 2 H 4 , and C 2 H 6 at 16.54, 8.30, 1.22, and 4.70 μmol g −1 h −1 , respectively, while maintaining stable activity over 16 h. The enhancement originates from intimate interfacial contact, stronger visible-light harvesting, faster charge transport, and increased accessible active sites. These results establish a practical heterostructure-design strategy for multi-electron photocatalytic CO 2 conversion.