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Bifunctional Fe─Ru─VC Catalyst for Energy Efficient Tandem Alkaline Electrolysis of Hydrazine and 4-nitrophenol. 双功能Fe─Ru─VC催化剂高效串联碱性电解肼和4-硝基苯酚。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202507522

Ali Mohammadi,Hanseung Kim,Mohammad Javad Arshia,Soobin Han,Abilash Sedhumadhavan,Reza Maleki,A T Ezhil Vilian,Arun Prakash Periasamy,Yun Suk Huh,Young-Kyu Han

{"title":"Bifunctional Fe─Ru─VC Catalyst for Energy Efficient Tandem Alkaline Electrolysis of Hydrazine and 4-nitrophenol.","authors":"Ali Mohammadi,Hanseung Kim,Mohammad Javad Arshia,Soobin Han,Abilash Sedhumadhavan,Reza Maleki,A T Ezhil Vilian,Arun Prakash Periasamy,Yun Suk Huh,Young-Kyu Han","doi":"10.1002/smll.202507522","DOIUrl":"https://doi.org/10.1002/smll.202507522","url":null,"abstract":"Alternate electrocatalytic reactions can turn pollutants into green fuels, offering an energy-efficient approach. Coupling hydrazine oxidation reaction (HzOR), with 4-nitrophenol hydrogenation (4-NPHR) is especially promising. Here, we report a bifunctional electrocatalyst composed of defect-rich Fe-Ru alloy clusters uniformly anchored on vanadium carbide (Fe─Ru─VC), synthesized via scalable ball milling and thermal annealing. Fe─Ru─VC exhibits excellent electrocatalytic activity toward both HzOR and 4-NPHR, requiring a low overpotential of 145 mV at 10 mA cm-2 and a favorable Tafel slope of 68.9 mV dec-1 for HzOR, with stability exceeding 90 h in 1M KOH. For 1 mM 4-NPHR, superior Fe-Ru-VC performance is achieved -7.2 mA cm-2 at 100 mV, highlighting its high efficiency. Furthermore, a paired H-cell electrolyzer (HzOR||4-NPHR) operates at only 200 mV to deliver 40 mA cm-2, underscoring its low energy demand. In situ Raman spectroscopy confirms the formation of Fe─Ru(OOH) as active sites, UV-Vis analysis confirms rapid 4-NP degradation, and DFT calculations demonstrate enhanced electronic interactions at the Ru─Fe junction, consistent with experimental observations. The outstanding activity is attributed to synergistic Fe-Ru interactions, the presence of zigzag edge defects, and the excellent conductivity of the VC support.","PeriodicalId":228,"journal":{"name":"Small","volume":"86 1","pages":"e07522"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Milliwatt-Scale Moisture-Induced Power Generation via Cation Intercalation in Sodium Vanadium Oxide Nanobelts. 毫瓦级水致发电技术在氧化钒钠纳米带中的应用。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202505223

Hyerim Baek,Minjae Song,Daewoong Kim,Dong Hyun Yoon,Kyung-Il Lee,Sangmin Jeon

{"title":"Milliwatt-Scale Moisture-Induced Power Generation via Cation Intercalation in Sodium Vanadium Oxide Nanobelts.","authors":"Hyerim Baek,Minjae Song,Daewoong Kim,Dong Hyun Yoon,Kyung-Il Lee,Sangmin Jeon","doi":"10.1002/smll.202505223","DOIUrl":"https://doi.org/10.1002/smll.202505223","url":null,"abstract":"A moisture-induced power generator (MPG) with exceptionally high-power output and extended operational stability is developed by systematically integrating three active materials: A LiCl -containing hydrogel, a perforated aluminum sheet, and NaV3O8 (NVO) nanobelts. The LiCl-containing hydrogel, due to its hygroscopic nature, maintains a stable moisture gradient and supplies charge carriers (Li+ ions). Simultaneously, the perforated aluminum sheet acts as the primary source of charge carriers (Al3+ ions) without generating oppositely charged ions, thereby preventing the degradation of the potential difference caused by ion migration. The NVO nanobelts undergo a reduction reaction through the intercalation of Li+ and Al3+ ions into their layered structure, effectively preventing reverse migration by resolving charge accumulation and generating Faradaic currents. Furthermore, their elongated structure enables the formation of a high-surface, conductive active layer through entanglement with carbon black nanoparticles, eliminating the need for binder materials. This systematic design achieves a maximum open-circuit voltage of 1.64 V, a short-circuit current of 10.44 mA cm-2, and a power density of 2.13 mW cm-2 at a load resistance of 200 Ω under 90% relative humidity. These results represent a record-high performance among reported MPGs, highlighting significant advancements in efficiency and durability, thereby enhancing the feasibility of MPGs for practical applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"1 1","pages":"e05223"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Controlling the Oxidation State of Copper in Metal-Organic Frameworks for CO Electroreduction to Acetate. CO电还原制乙酸金属有机骨架中铜的氧化态控制。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202509324

Ying Jiao,Senlin Chu,Nengji Liu,Bo-Xin Zhang,Yang Hou,Xiang Zhao

引用次数: 0

Direct Observation of Spherulitic Covalent Triazine Frameworks Grown in Hot Superacid Matrices. 在热超强酸基质中生长球形共价三嗪骨架的直接观察。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202509494

Tianhao Fang,Yifeng Xing,Huimin Wu,Duan Gao,Xiaomin Xu,Zhenghua Zhang,Huai-Zhen Wang,Zhen Chen

{"title":"Direct Observation of Spherulitic Covalent Triazine Frameworks Grown in Hot Superacid Matrices.","authors":"Tianhao Fang,Yifeng Xing,Huimin Wu,Duan Gao,Xiaomin Xu,Zhenghua Zhang,Huai-Zhen Wang,Zhen Chen","doi":"10.1002/smll.202509494","DOIUrl":"https://doi.org/10.1002/smll.202509494","url":null,"abstract":"As emerging porous crystalline polymers, 2D covalent organic frameworks present exclusively in macroscopic forms of polycrystalline powders, single crystals, or thin films. Here, spherulitic 2D covalent triazine frameworks (CTFs) grown in hot superacid matrices are grown, which exhibit a typical Maltese cross pattern of light extinction. A structural evolution from small-angle branched nanofibrils to a core-shell hemispherical geometry is real-time recorded by in situ microscopies and spectroscopies. Time-resolved imaging analysis on spherulitic growth unveils a nonclassical crystallization process, which involves a secondary nucleation-elongation mechanism coupled with amorphous-to-crystalline transition. Furthermore, fluorine doping into CTF enables acceleration of 2D template polymerization and shell formation to develop size-tunable spherulites, with the optimal size up to ≈48 µm in diameter. This work provides unique insights into 2D polymerization and crystallization processes via in situ characterization and demonstrates an unprecedented form of CTF crystallites, which are potentially used as ion sensors and storage.","PeriodicalId":228,"journal":{"name":"Small","volume":"8 1","pages":"e09494"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fluorine-Mediated Carbon Doping in Boron Nitride: Atomic-Level Interface Engineering for Balancing Microwave Absorption and Thermal Management. 氮化硼中氟介导的碳掺杂：平衡微波吸收和热管理的原子级界面工程。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202506851

Zhangwen Xie,Yufei Tang,Yagang Zhang,Wanxing Zheng,Yani Sun,Huan Zhong,Shiyu Zhang,Qingnan Meng,Kang Zhao

{"title":"Fluorine-Mediated Carbon Doping in Boron Nitride: Atomic-Level Interface Engineering for Balancing Microwave Absorption and Thermal Management.","authors":"Zhangwen Xie,Yufei Tang,Yagang Zhang,Wanxing Zheng,Yani Sun,Huan Zhong,Shiyu Zhang,Qingnan Meng,Kang Zhao","doi":"10.1002/smll.202506851","DOIUrl":"https://doi.org/10.1002/smll.202506851","url":null,"abstract":"The advancement of high-density integrated electronics urgently demands materials that integrate efficient thermal management and microwave absorption. However, conventional design strategies that often rely on materials with multi-component composites face a trade-off between these properties, and a lack of microwave absorption effectiveness study in the polymer matrix. Herein, a fluorine-mediated carbon doping in boron nitride (C-F-BN) is designed to achieve atomic-level interface engineering. Fluoride induces the formation of polarized C─F bonds and promotes ordered sp2-carbon incorporation, which well preserves the BN lattice integrity while establishing strong polarization sites. The resulting C-F-BN shows exceptional microwave absorption with a reflection loss of -43 dB at 2 mm thickness, compared to that of only carbon doping in BN, achieving an effective absorption bandwidth of 3.52 GHz and a remarkable absorption efficiency index of 35 dB· GHz mm-1. The maintained BN crystallinity, ordered sp2-carbon conversion, and enhanced interfacial compatibility between C-F-BN and polyvinyl alcohol (PVA) enable PVA/C-F-BN composites to attain higher through-plane thermal conductivity (0.2599 W·m-1·K-1) at a lower filler loading (5 wt.%). Moreover, the composite exhibits a broader absorption bandwidth of 3.84 GHz with a reflection loss of -32 dB. The design concept offers a feasible route to multifunctional materials for advanced electronic packaging.","PeriodicalId":228,"journal":{"name":"Small","volume":"31 1","pages":"e06851"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tailoring Surface Chemistry of Ti3C2Nx MXene for Superior H+, Li+, and Na+ Storage via Molten Salt-Derived N-Termination. 熔盐衍生n端对Ti3C2Nx MXene表面化学修饰的影响

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202508556

Tiezhu Guo,Wenfei Wei,Jiali Chai,Yuchuan Ren,Murat Yilmaz,Azim Uddin,Andreu Cabot,Di Zhou

{"title":"Tailoring Surface Chemistry of Ti3C2Nx MXene for Superior H+, Li+, and Na+ Storage via Molten Salt-Derived N-Termination.","authors":"Tiezhu Guo,Wenfei Wei,Jiali Chai,Yuchuan Ren,Murat Yilmaz,Azim Uddin,Andreu Cabot,Di Zhou","doi":"10.1002/smll.202508556","DOIUrl":"https://doi.org/10.1002/smll.202508556","url":null,"abstract":"2D transition metal carbides and nitrides (MXene) are promising candidates for next-generation electrode materials due to their high electrical conductivity, large specific capacity/capacitance, and tunable surface chemistry. Nitrogen-doped MXene, in particular, have shown excellent electrochemical energy storage performance. However, the low and uneven nitrogen content has hindered both their performance and understanding of how N-terminal groups affect cation storage. This study successfully synthesizes N-terminated Ti3C2Nx via ion-exchange reactions in a hydrogen-containing argon atmosphere and investigates its energy storage behavior for H⁺, Li⁺, and Na⁺ ions. Ti3C2Nx shows outstanding H⁺ storage with a capacitance of 471 F g-1, while Li⁺ and Na⁺ storage exhibit a prominent intercalation mechanism. The Ti3C2Nx electrode delivers stable capacities of 209 mAh g-1 for Li⁺ and 79 mAh g-1 for Na⁺ after rate cycling, indicating good rate capability and reversibility. Combining density functional theory calculations with experimental data, this study reveals the correlations between adsorption energy, binding energy, and electronic density of states, highlighting the importance of real-gap distance in efficient cation intercalation, offering guidance for the design of MXene for H⁺, Li⁺, and Na⁺ storage.","PeriodicalId":228,"journal":{"name":"Small","volume":"20 1","pages":"e08556"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Piezocatalysis-Enabled High-Efficiency Hydrogen Evolution with Single-Atom Platinum on MoS2 Nanoflowers. 单原子铂在MoS2纳米花上的压电催化高效析氢。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202508162

Yu-Ming Chen,Yu-Ching Chen,Kuang-Yuan Tu,Yi-Dong Lin,Yan-Gu Lin,Hsun-Yen Lin,Samiksha Bajaj,Jyh Ming Wu

{"title":"Piezocatalysis-Enabled High-Efficiency Hydrogen Evolution with Single-Atom Platinum on MoS2 Nanoflowers.","authors":"Yu-Ming Chen,Yu-Ching Chen,Kuang-Yuan Tu,Yi-Dong Lin,Yan-Gu Lin,Hsun-Yen Lin,Samiksha Bajaj,Jyh Ming Wu","doi":"10.1002/smll.202508162","DOIUrl":"https://doi.org/10.1002/smll.202508162","url":null,"abstract":"The advent of single-atom catalysts (SACs) has revolutionized catalysis, delivering outstanding performance in diverse chemical reactions. This study introduces a novel piezoelectric catalytic system employing single-atom platinum-modified MoS2 nanoflowers (NFs) for enhanced hydrogen evolution reactions (HER). High-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) identifies single-atom platinum as bright dots, while X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analyses verify its oxidation state and radial distance. Piezoresponse force microscopy (PFM) confirms increased piezoresponse amplitude due to structural asymmetry from platinum modification. Time-resolved photoluminescence (TRPL) reveals an extended carrier lifetime of 5.7 ns, while the modified catalyst (SA-Pt-01, MoS2 NFs with 1 wt.% Pt) achieves a fourfold increase in hydrogen production efficiency, reaching 2206.15 µmol·g-1·h-1. Notably, SA-Pt-1 generates 7786.9 µmol·g-1 in 12 h, showcasing sustained performance. Electron paramagnetic resonance (EPR) detects stronger •OH radical signals, indicating increased reactive availability. Density functional theory (DFT) simulations show that single-atom Pt incorporation enhances adsorption energy and reduces energy barriers for hydrogen production. These findings underscore the potential of single-atom Pt-modified MoS2 NFs as efficient, sustainable catalysts for clean hydrogen energy applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"22 1","pages":"e08162"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synergistic Effects of Cu(OH)2-CuO Anodes for Multiple-Step Energy Storage of Li-Ion Microbatteries. Cu(OH)2-CuO阳极在锂离子微电池多级储能中的协同效应

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202508106

Srinivasan Alagar,Hyunki Kim,Joonhee Moon,Jun Kim,Chandra Sekhar Rout,Han Seul Kim,Sang Mun Jeong

{"title":"Synergistic Effects of Cu(OH)2-CuO Anodes for Multiple-Step Energy Storage of Li-Ion Microbatteries.","authors":"Srinivasan Alagar,Hyunki Kim,Joonhee Moon,Jun Kim,Chandra Sekhar Rout,Han Seul Kim,Sang Mun Jeong","doi":"10.1002/smll.202508106","DOIUrl":"https://doi.org/10.1002/smll.202508106","url":null,"abstract":"Lithium-ion microbatteries (LIMBs) face challenges in achieving high power density without compromising energy density, due to limitations in assembly and kinetics. By overcoming LIMB electrode fabricated using a laser-assisted method, which significantly improves assembly precision and enhances reaction kinetics, the first anodization of Cu(OH)2-CuO nanoneedle hybrids on Cu foil for a LIB anode is reported. By resolving the limitations of previous metal-hydroxide electrodes associated with conventional conversion reactions, the novel anode achieves an unprecedently-high initial capacity of 3065 mAh g-1 which clearly exceeds the theoretical limit. X-ray Photoelectron Spectroscopy, Transmission Electron Microscopy, and in-situ Raman analysis revealed the nanoscale Cu-particles and LiOH in high-voltage reactions, alongside CuxHy, Li2O, and LiH in low-voltage hydride reactions. AIMD simulations additionally revealed the underlying atomistic mechanism. An in-plane LIMB using a laser-assisted method is further engineered, featuring in prelithiated Cu(OH)2-CuO as the anode and LiNi0.8Mn0.1Co0.1O2 as the cathode. This LIMB operates between 2.0 and 4.5 V, delivering a reversible capacity of 6.61 mAh cm-2 at 20 µA cm-2 and retaining over 83% capacity after 500 cycles. This work advances overall understanding of lithium storage and offers key insights for the design of next-generation LIMBs.","PeriodicalId":228,"journal":{"name":"Small","volume":"104 1","pages":"e08106"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering of Chain Extender Flexibility and Hierarchical Hydrogen Bonding Toward Ultra-Low-Temperature Poly(Urethane-Urea) Elastomers with Exceptional Toughness. 具有特殊韧性的超低温聚（聚氨酯-尿素）弹性体扩链剂柔韧性和层次式氢键工程。

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202509686

Kelei Luo,Xiaoyue Wang,Qian Dou,Pengrui Cao,Jing Yang,Lihe Guo,Qi Guo,Song Li,Qihua Wang,Tingmei Wang,Liming Tao

{"title":"Engineering of Chain Extender Flexibility and Hierarchical Hydrogen Bonding Toward Ultra-Low-Temperature Poly(Urethane-Urea) Elastomers with Exceptional Toughness.","authors":"Kelei Luo,Xiaoyue Wang,Qian Dou,Pengrui Cao,Jing Yang,Lihe Guo,Qi Guo,Song Li,Qihua Wang,Tingmei Wang,Liming Tao","doi":"10.1002/smll.202509686","DOIUrl":"https://doi.org/10.1002/smll.202509686","url":null,"abstract":"The demand for elastomeric materials with exceptional mechanical properties at low temperatures is increasingly growing. However, meeting these requirements remains a significant challenge to date. The high strength and toughness of many PTMEG-based elastomers are compromised at low temperatures. The ordered nature of their molecular chains leads to (semi-)crystallization of the soft segments, preventing substantial recovery. In this study, a series of hydroxyl terminated polybutadiene-based polyurethane (HTPB-PU) elastomers (HPUs) with balanced rigidity and flexibility are synthesized by modulating the interplay between rigid (urethane and urea bonds combined with aryl groups) and flexible molecular segments (HTPB). Hierarchical hydrogen bonding and aryl π-π stacking form rigid nanostructured domains, together with the large polarity difference and absence of hydrogen bonds between the soft and hard segments of HPUs, resulting in pronounced microphase separation. The rigid nanostructured domains disrupt the regular alignment of HTPB chains, thereby enabling the material to maintain exceptional ductility at -70 °C. Consequently, the HPUs exhibit remarkable elongation at break (842.6 ± 7.4%), exceptional fracture toughness (254.1 ± 16.0 MJ m-3), as well as excellent tear resistance, oil resistance, solvent resistance, and fatigue resistance at -70 °C. These findings provide a promising pathway for designing next-generation elastomers for extreme environments.","PeriodicalId":228,"journal":{"name":"Small","volume":"47 1","pages":"e09686"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229150","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancement of Persulfate Activation via Dual-Site Coordination and Electron Redistribution at Co─O─Zr Metal-Support Interfaces for Photo-Fenton-Like Reactions. Co─O─Zr金属载体界面上的双位配位和电子重分布增强过硫酸盐活化光- fenton类反应

IF 13.3 2区材料科学

Small Pub Date : 2025-10-06 DOI: 10.1002/smll.202506875

Jiajie Xu,Tenghui Jin,Wei Qu,Kaizhou Huang,Zhiyu Liu,Ping Zhang,Jiaping Paul Chen

{"title":"Enhancement of Persulfate Activation via Dual-Site Coordination and Electron Redistribution at Co─O─Zr Metal-Support Interfaces for Photo-Fenton-Like Reactions.","authors":"Jiajie Xu,Tenghui Jin,Wei Qu,Kaizhou Huang,Zhiyu Liu,Ping Zhang,Jiaping Paul Chen","doi":"10.1002/smll.202506875","DOIUrl":"https://doi.org/10.1002/smll.202506875","url":null,"abstract":"Development of high-performance photocatalysts for persulfate activation is often limited by rapid electron-hole recombination and insufficient quantum efficiency. To overcome the challenges, electronic metal-support interaction (EMSI) structure is designed. The innovative structure has several key benefits: recombination rates are significantly reduced, charge separation is enhanced, and content of active sites and intrinsic catalytic activity are increased. ZrO2/Co3O4 bimetallic oxides featuring a synergistic Co─O─Zr EMSI coordination are synthesized via a sol-gel method. Strong EMSI effects markedly modulate and stabilize the Co 3d electronic structure, creating an electron-rich center on Co sites to promote persulfate activation, and an electron-deficient center on Zr sites to adsorb atrazine. The Gibbs free energy analysis reveals that Zr incorporation reduces the overpotential of oxygen evolution reaction, thereby facilitating electron transfer, promoting hole consumption and suppressing charge recombination. More importantly, it promotes the generation of reactive oxygen species-predominantly via a singlet oxygen (1O2)-dominated non-radical mechanism. The optimized catalyst achieves 97.3% degradation of atrazine (a model compound) under visible light, outperforming commercial catalysts (e.g., 4.5-fold of Co3O4). The work elucidates the cooperative mechanism of dual-site engineering and EMSI-mediated electron redistribution, providing a rational strategy for designing efficient photocatalysts toward sustainable advanced oxidation processes.","PeriodicalId":228,"journal":{"name":"Small","volume":"24 1","pages":"e06875"},"PeriodicalIF":13.3,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0