Pub Date : 2026-01-11DOI: 10.1016/j.apsusc.2026.165898
Hao Zhang , Juan Yu , Tian Wang , Shaojie Li , Gang Wang , Jingsen Yue , Tianxin Kang
Aqueous zinc-ion batteries (AZIBs) based on manganese oxide (MnO2) hold great promise for grid-scale energy storage. However, manganese-based cathode materials still face challenges such as low intrinsic electronic conductivity, sluggish Zn2+ diffusion kinetics, and structural degradation caused by manganese dissolution during cycling. To address these issues, this study proposes a strategy for the in-situ electrochemical oxidation synthesis of MnO2 cathode materials with enlarged interlayer spacing. Specifically, a MnO precursor was first subjected to mechanical activation to induce structural distortions, including surface defects, dislocations, and lattice expansion. Subsequently, the activated MnO was electrochemically oxidized in situ to form a layered MnO2, simultaneously achieving self-assembly with conductive graphite. The resulting composite material possesses a large interlayer spacing of 0.93 nm, which significantly facilitates the reversible (de)intercalation of Zn2+. Electrochemical tests demonstrate that this cathode delivers a reversible specific capacity of 74.5mAh g−1 at a high current density of 10 A g−1 and exhibits an outstanding capacity retention of 90 % after 1350 cycles. This work not only provides deeper insights into the formation mechanism of anion-close-packed manganese oxides but also offers a novel strategy for designing high-performance cathode materials for AZIBs.
基于氧化锰（MnO2）的水锌离子电池（azib）在电网规模的储能方面具有很大的前景。然而，锰基正极材料仍然面临着固有电导率低、Zn2+扩散动力学缓慢以及循环过程中锰溶解导致的结构降解等挑战。为了解决这些问题，本研究提出了一种扩大层间距的二氧化锰正极材料的原位电化学氧化合成策略。具体来说，MnO前驱体首先受到机械激活来诱导结构畸变，包括表面缺陷、位错和晶格膨胀。随后，将活化后的二氧化锰原位电化学氧化形成层状二氧化锰，同时实现与导电石墨的自组装。复合材料的层间距为0.93 nm，有利于Zn2+的可逆（脱）插层。电化学测试表明，该阴极在10 a g−1的高电流密度下提供了74.5mAh g−1的可逆比容量，并且在1350次循环后表现出优异的90 %的容量保持率。这项工作不仅为阴离子紧密堆积的锰氧化物的形成机制提供了更深入的见解，而且为设计高性能azib正极材料提供了一种新的策略。
{"title":"In situ formation and performance of layered MnO2 cathode materials with large interlayer Spacing: A mechano-electrochemical oxidation strategy","authors":"Hao Zhang , Juan Yu , Tian Wang , Shaojie Li , Gang Wang , Jingsen Yue , Tianxin Kang","doi":"10.1016/j.apsusc.2026.165898","DOIUrl":"10.1016/j.apsusc.2026.165898","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs) based on manganese oxide (MnO<sub>2</sub>) hold great promise for grid-scale energy storage. However, manganese-based cathode materials still face challenges such as low intrinsic electronic conductivity, sluggish Zn<sup>2+</sup> diffusion kinetics, and structural degradation caused by manganese dissolution during cycling. To address these issues, this study proposes a strategy for the in-situ electrochemical oxidation synthesis of MnO<sub>2</sub> cathode materials with enlarged interlayer spacing. Specifically, a MnO precursor was first subjected to mechanical activation to induce structural distortions, including surface defects, dislocations, and lattice expansion. Subsequently, the activated MnO was electrochemically oxidized in situ to form a layered MnO<sub>2</sub>, simultaneously achieving self-assembly with conductive graphite. The resulting composite material possesses a large interlayer spacing of 0.93 nm, which significantly facilitates the reversible (de)intercalation of Zn<sup>2+</sup>. Electrochemical tests demonstrate that this cathode delivers a reversible specific capacity of 74.5mAh g<sup>−1</sup> at a high current density of 10 A g<sup>−1</sup> and exhibits an outstanding capacity retention of 90 % after 1350 cycles. This work not only provides deeper insights into the formation mechanism of anion-close-packed manganese oxides but also offers a novel strategy for designing high-performance cathode materials for AZIBs.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165898"},"PeriodicalIF":6.9,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956540","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}
Pub Date : 2026-01-11DOI: 10.1016/j.apsusc.2026.165885
Mengmeng Li , Zhisen Li , Chong Peng , Tiezhu Zhang , Tao E , Shuyi Yang
In the electrochemically activated persulfate (PS) advanced oxidation process, overcoming the efficiency limitation in converting dissolved oxygen into active radicals remains a major challenge. Therefore, this study designed an anode–cathode synergistic strategy and fabricated CeO2/BC/NF as the core cathode catalyst via a one-step hydrothermal method. This system achieved a tetracycline (TC) degradation efficiency of 90.96 % within 60 min and retained over 85 % of its initial activity after 10 cycles. Mechanistic investigations reveal that the performance enhancement stems from the innovative coupling and utilization of the anodic oxygen evolution reaction (OER) and the cathodic oxygen reduction reaction (ORR). Specifically, O2 generated at the anode is rapidly transported to the CeO2/BC/NF cathode surface, where it is efficiently converted into superoxide radicals (·O2-) through a single‑electron reduction pathway. This anode‑driven, cathode‑executed “oxygen‑supply-oxygen‑consumption” closed loop acts synergistically with the PS activation pathway at the cathode (which generates sulfate radicals and other species), jointly establishing a rich radical reservoir and thereby significantly boosting the overall oxidation capacity. By shifting the optimization focus from the conventional single‑electrode or single‑pathway level to the system‑level concept of inter‑electrode synergy, this study provides a new paradigm for enhancing electrochemical oxidation technologies.
{"title":"Deciphering anode-cathode synergy via the interfacial role of CeO2/BC/NF to efficiently degrade tetracycline","authors":"Mengmeng Li , Zhisen Li , Chong Peng , Tiezhu Zhang , Tao E , Shuyi Yang","doi":"10.1016/j.apsusc.2026.165885","DOIUrl":"10.1016/j.apsusc.2026.165885","url":null,"abstract":"<div><div>In the electrochemically activated persulfate (PS) advanced oxidation process, overcoming the efficiency limitation in converting dissolved oxygen into active radicals remains a major challenge. Therefore, this study designed an anode–cathode synergistic strategy and fabricated CeO<sub>2</sub>/BC/NF as the core cathode catalyst via a one-step hydrothermal method. This system achieved a tetracycline (TC) degradation efficiency of 90.96 % within 60 min and retained over 85 % of its initial activity after 10 cycles. Mechanistic investigations reveal that the performance enhancement stems from the innovative coupling and utilization of the anodic oxygen evolution reaction (OER) and the cathodic oxygen reduction reaction (ORR). Specifically, O<sub>2</sub> generated at the anode is rapidly transported to the CeO<sub>2</sub>/BC/NF cathode surface, where it is efficiently converted into superoxide radicals (·O<sub>2</sub><sup>-</sup>) through a single‑electron reduction pathway. This anode‑driven, cathode‑executed “oxygen‑supply-oxygen‑consumption” closed loop acts synergistically with the PS activation pathway at the cathode (which generates sulfate radicals and other species), jointly establishing a rich radical reservoir and thereby significantly boosting the overall oxidation capacity. By shifting the optimization focus from the conventional single‑electrode or single‑pathway level to the system‑level concept of inter‑electrode synergy, this study provides a new paradigm for enhancing electrochemical oxidation technologies.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165885"},"PeriodicalIF":6.9,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947509","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}
Pub Date : 2026-01-11DOI: 10.1016/j.apsusc.2026.165881
Xiaofang Wen , Hongcan Lou , Zheng Li , Jiehao Xie , Zirui Qin , Xingkun Chen , Yuan Tan , Nian Lei , Wei Lu , Yunjie Ding
The development of efficient catalysts for the selective hydrogenation of dimethyl oxalate (DMO) to high-value oxygenates is of great industrial importance. This study presents a systematic investigation into the promotional effect of gallium (Ga) on Cu/SiO2 catalysts for tailoring product selectivity in DMO hydrogenation. A series of GaxCu30/SiO2 catalysts with varying Ga loadings (x = 0.5, 1, 3 wt%) were synthesized via the ammonia evaporation method. With a moderate Ga doping of 0.5 wt%, the Ga0.5Cu30/SiO2 catalyst achieved an exceptional ethylene glycol (EG) yield of 74 %, which is three times higher than its Ga-free counterpart (23 %). Further increases in Ga loading to 1 and 3 wt% redirected the reaction pathway, steering the selectivity towards ethanol (ET, 81 %) and 2-methoxyethanol (MT, 54 %), respectively. Characterization by N2O titration, XRD, XPS, in situ FT-IR and H2-TPR revealed that Ga incorporation fine-tunes the synergy between metallic Cu0 (for H2 dissociation) and Cu+ sites (for C=O bond polarization). Concurrently, the generated surface acid sites facilitate subsequent dehydration and hydrogenolysis steps. Consequently, the catalytic performance is directly correlated with the evolution of Cu valence states and surface acidity. This work provides a rational strategy for designing multifunctional catalysts for the selective synthesis of target chemicals from DMO.
{"title":"Tuning product selectivity in dimethyl oxalate hydrogenation via Ga-promoted Cu/SiO2 catalysts: the interplay between Cu+/Cu0 sites and surface acidity","authors":"Xiaofang Wen , Hongcan Lou , Zheng Li , Jiehao Xie , Zirui Qin , Xingkun Chen , Yuan Tan , Nian Lei , Wei Lu , Yunjie Ding","doi":"10.1016/j.apsusc.2026.165881","DOIUrl":"10.1016/j.apsusc.2026.165881","url":null,"abstract":"<div><div>The development of efficient catalysts for the selective hydrogenation of dimethyl oxalate (DMO) to high-value oxygenates is of great industrial importance. This study presents a systematic investigation into the promotional effect of gallium (Ga) on Cu/SiO<sub>2</sub> catalysts for tailoring product selectivity in DMO hydrogenation. A series of Ga<sub>x</sub>Cu<sub>30</sub>/SiO<sub>2</sub> catalysts with varying Ga loadings (x = 0.5, 1, 3 wt%) were synthesized via the ammonia evaporation method. With a moderate Ga doping of 0.5 wt%, the Ga<sub>0.5</sub>Cu<sub>30</sub>/SiO<sub>2</sub> catalyst achieved an exceptional ethylene glycol (EG) yield of 74 %, which is three times higher than its Ga-free counterpart (23 %). Further increases in Ga loading to 1 and 3 wt% redirected the reaction pathway, steering the selectivity towards ethanol (ET, 81 %) and 2-methoxyethanol (MT, 54 %), respectively. Characterization by N<sub>2</sub>O titration, XRD, XPS, in situ FT-IR and H<sub>2</sub>-TPR revealed that Ga incorporation fine-tunes the synergy between metallic Cu<sup>0</sup> (for H<sub>2</sub> dissociation) and Cu<sup>+</sup> sites (for C=O bond polarization). Concurrently, the generated surface acid sites facilitate subsequent dehydration and hydrogenolysis steps. Consequently, the catalytic performance is directly correlated with the evolution of Cu valence states and surface acidity. This work provides a rational strategy for designing multifunctional catalysts for the selective synthesis of target chemicals from DMO.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165881"},"PeriodicalIF":6.9,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956545","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}
Pub Date : 2026-01-10DOI: 10.1016/j.apsusc.2026.165879
Fan Zhang, Xiaomin Qiu, Hongxin Wang, Yujiao Bi, Zhijie Shang, Hongbing Song
The efficient treatment of oily wastewater remains a critical challenge in chemical engineering due to the limitations of conventional separation technologies such as adsorption, flotation, and gravity separation. Here, we report a strategy to regulate both surface chemistry and micro–nano roughness of poly(ionic liquid)s (PIL-s) to achieve high-performance oil–water separation. Dual-cationic ionic liquid monomers were polymerized via Friedel–Crafts reactions with different crosslinking and co-crosslinking agents, yielding PILs with tunable wettability ranging from superhydrophilic–oleophobic to hydrophobic–oleophilic. The optimized membranes achieved separation efficiencies above 99 % and fluxes up to 7324 L·m−2·h−1, while maintaining stable performance over 20 consecutive cycles. Mechanistic analysis based on Young, Wenzel, and Cassie–Baxter models revealed that the synergistic interplay between surface energy and structural roughness governs wettability transitions and separation behavior. This work demonstrates a versatile material platform with potential for scalable oily wastewater treatment, offering both high throughput and durability.
{"title":"Regulating the surface structure of poly(ionic liquid)s for high-performance oil-water separation","authors":"Fan Zhang, Xiaomin Qiu, Hongxin Wang, Yujiao Bi, Zhijie Shang, Hongbing Song","doi":"10.1016/j.apsusc.2026.165879","DOIUrl":"10.1016/j.apsusc.2026.165879","url":null,"abstract":"<div><div>The efficient treatment of oily wastewater remains a critical challenge in chemical engineering due to the limitations of conventional separation technologies such as adsorption, flotation, and gravity separation. Here, we report a strategy to regulate both surface chemistry and micro–nano roughness of poly(ionic liquid)s (PIL-s) to achieve high-performance oil–water separation. Dual-cationic ionic liquid monomers were polymerized via Friedel–Crafts reactions with different crosslinking and co-crosslinking agents, yielding PILs with tunable wettability ranging from superhydrophilic–oleophobic to hydrophobic–oleophilic. The optimized membranes achieved separation efficiencies above 99 % and fluxes up to 7324 L·m<sup>−2</sup>·h<sup>−1</sup>, while maintaining stable performance over 20 consecutive cycles. Mechanistic analysis based on Young, Wenzel, and Cassie–Baxter models revealed that the synergistic interplay between surface energy and structural roughness governs wettability transitions and separation behavior. This work demonstrates a versatile material platform with potential for scalable oily wastewater treatment, offering both high throughput and durability.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165879"},"PeriodicalIF":6.9,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956543","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}
Pub Date : 2026-01-10DOI: 10.1016/j.apsusc.2026.165891
Jinbo Xue , Jiahao Niu , Jinlong Li , Wenjie Wang , Qianqian Shen , Yuxing Yan , Xiao Lin
Although photocatalytic technology is considered an efficient and green solution for treating hexavalent chromium (Cr (VI)), the difficulty in recovering powder catalysts limits its practical application. In this study, a novel composite photocatalyst TiO2/Vo-Bi4Ti3O12 (TiO2/Vo-BTO) was in situ constructed on an industrial titanium mesh. Utilizing water flow pressure to induce a piezoelectric polarization field in Vo- Bi4Ti3O12, promoting photogenerated charge separation to achieve efficient photoreduction of Cr(VI) to Cr(III). The introduction of oxygen vacancies in Bi4Ti3O12 enhances the electron localization around the Ti atoms, increases the rigidity of the Ti–O bonds, and causes lattice distortion (octahedral tilt), hindering domain reversal and thus stabilizing the polarization field in a turbulent environment. The optimized TiO2/Vo-BTO catalyst exhibited excellent photocatalytic reduction performance in a fixed-bed reactor, achieving a 99% reduction rate of Cr (VI) within 1.5 h, with an apparent reaction kinetic constant kobs as high as 2.859 h−1. The piezoelectric-defect synergistic regulation strategy proposed in this study offers a novel approach for developing highly efficient, stable, and recyclable photocatalytic systems. It provides significant guidance for advancing the practical application of photocatalytic technology in wastewater treatment.
{"title":"Water Flow-Induced piezoelectric polarization Synergized with oxygen vacancies for enhanced photocatalytic reduction of Cr (VI) over TiO2/Vo-Bi4Ti3O12","authors":"Jinbo Xue , Jiahao Niu , Jinlong Li , Wenjie Wang , Qianqian Shen , Yuxing Yan , Xiao Lin","doi":"10.1016/j.apsusc.2026.165891","DOIUrl":"10.1016/j.apsusc.2026.165891","url":null,"abstract":"<div><div>Although photocatalytic technology is considered an efficient and green solution for treating hexavalent chromium (Cr (VI)), the difficulty in recovering powder catalysts limits its practical application. In this study, a novel composite photocatalyst TiO<sub>2</sub>/Vo-Bi<sub>4</sub>Ti<sub>3</sub>O<sub>12</sub> (TiO<sub>2</sub>/Vo-BTO) was in situ constructed on an industrial titanium mesh. Utilizing water flow pressure to induce a piezoelectric polarization field in Vo- Bi<sub>4</sub>Ti<sub>3</sub>O<sub>12</sub>, promoting photogenerated charge separation to achieve efficient photoreduction of Cr(VI) to Cr(III). The introduction of oxygen vacancies in Bi<sub>4</sub>Ti<sub>3</sub>O<sub>12</sub> enhances the electron localization around the Ti atoms, increases the rigidity of the Ti–O bonds, and causes lattice distortion (octahedral tilt), hindering domain reversal and thus stabilizing the polarization field in a turbulent environment. The optimized TiO<sub>2</sub>/Vo-BTO catalyst exhibited excellent photocatalytic reduction performance in a fixed-bed reactor, achieving a 99% reduction rate of Cr (VI) within 1.5 h, with an apparent reaction kinetic constant kobs as high as 2.859 h<sup>−1</sup>. The piezoelectric-defect synergistic regulation strategy proposed in this study offers a novel approach for developing highly efficient, stable, and recyclable photocatalytic systems. It provides significant guidance for advancing the practical application of photocatalytic technology in wastewater treatment.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165891"},"PeriodicalIF":6.9,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947517","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}
The synthesis of high-performance A15-phase Nb3Sn films at temperatures compatible with copper substrates (< 800 °C) remains a significant challenge for next-generation superconducting radio-frequency (SRF) cavities. Conventional methods require high temperatures, which precludes direct deposition on Cu. This study demonstrates a low-temperature deposition strategy using high-power impulse magnetron sputtering (HiPIMS), which provides highly energetic ions to enhance adatom mobility and crystallization kinetics. By systematically optimizing the substrate temperature and bias voltage, we achieved the direct growth of high-quality Nb3Sn films on sapphire substrates. Remarkably, the film deposited at 750 °C with a −50 V bias attained a high superconducting transition temperature (Tc) of 17.43 K without any post-annealing—a value that is among the highest reported for films prepared below 800 °C. Furthermore, this study investigated the influence of particles with different energy levels on the properties of Nb3Sn films and elucidated the underlying mechanisms. This work establishes HiPIMS as a potent technique for low-temperature fabrication of Nb3Sn coatings, paving the way for their integration into cost-effective and high-performance Cu-based SRF cavities.
{"title":"Fabrication of high-Tc Nb3Sn films below 800 °C: A HiPIMS approach enabling copper-cavity applications","authors":"Yaxu Wu, Tianwei Sun, Yuanshu Zou, Jiahao Zhang, Langping Wang, Xiaofeng Wang","doi":"10.1016/j.apsusc.2026.165895","DOIUrl":"10.1016/j.apsusc.2026.165895","url":null,"abstract":"<div><div>The synthesis of high-performance A15-phase Nb<sub>3</sub>Sn films at temperatures compatible with copper substrates (< 800 °C) remains a significant challenge for next-generation superconducting radio-frequency (SRF) cavities. Conventional methods require high temperatures, which precludes direct deposition on Cu. This study demonstrates a low-temperature deposition strategy using high-power impulse magnetron sputtering (HiPIMS), which provides highly energetic ions to enhance adatom mobility and crystallization kinetics. By systematically optimizing the substrate temperature and bias voltage, we achieved the direct growth of high-quality Nb<sub>3</sub>Sn films on sapphire substrates. Remarkably, the film deposited at 750 °C with a −50 V bias attained a high superconducting transition temperature (<em>T</em><sub>c</sub>) of 17.43 K without any post-annealing—a value that is among the highest reported for films prepared below 800 °C. Furthermore, this study investigated the influence of particles with different energy levels on the properties of Nb<sub>3</sub>Sn films and elucidated the underlying mechanisms. This work establishes HiPIMS as a potent technique for low-temperature fabrication of Nb<sub>3</sub>Sn coatings, paving the way for their integration into cost-effective and high-performance Cu-based SRF cavities.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165895"},"PeriodicalIF":6.9,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956579","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}
Pt/PDMS (polydimethylsiloxane) flexible thin-film neural electrodes represent a promising platform for chronic neural signal acquisition and neuromodulation. However, inherent mechanical and electrochemical instability arises from insufficient interfacial adhesion at the metal-polymer boundary, manifesting as progressive delamination and impedance drift under cyclic mechanical loading. To address these challenges, we present a synergistic engineering strategy integrating three complementary approaches: geometric optimization of electrode array configurations, femtosecond laser-processed micro/nanostructured mechanical interlocks, and polymer matrix toughening through hexane-induced PDMS crosslinking modification. Finite element analysis and cyclic bending tests indicate that the optimized circular electrode array effectively distributes stress and alleviates stress concentration. Parametric Geometry Optimization enables active control of serpentine unit geometry, suppressing local stress and outperforming conventional designs under multi-axis loads.Furthermore, femtosecond laser processing creates periodic micro-nanostructures that form mechanical interlocks, significantly enhancing interfacial adhesion. Micro-Nano Interfacial Interlocking combines surface patterning with substrate modification to achieve robust adhesion, overcoming modulus mismatch. Additionally, hexane-modified PDMS improves polymer toughness, reinforcing the reliability of the interlocking structure. These innovations are integrated into a multi-scale design that synergizes geometric and material engineering, providing a comprehensive solution for long-term reliability of flexible implantable electrodes. This integrated approach increases Pt/PDMS interface bonding strength to 4.412 MPa, 9.74 times higher than that of the untreated samples, while reducing impedance fluctuations after cyclic bending (500 cycles, 80%) to 18.3%. These advancements collectively enable a new paradigm in durable flexible bioelectronics, where multiscale structural engineering synergistically enhances both mechanical robustness and functional reliability in chronic implantation scenarios.
{"title":"A synergistic strategy for enhancing the stability of Pt/PDMS flexible electrodes: integration of array geometry optimization and interfacial mechanical interlocking","authors":"Liangping Ma, Ban Chen, Wanchen Zhang, Tengyu Guo, Xiaowei Han, Donghui Wang, Hongshui Wang, Chunyong Liang","doi":"10.1016/j.apsusc.2026.165854","DOIUrl":"https://doi.org/10.1016/j.apsusc.2026.165854","url":null,"abstract":"Pt/PDMS (polydimethylsiloxane) flexible thin-film neural electrodes represent a promising platform for chronic neural signal acquisition and neuromodulation. However, inherent mechanical and electrochemical instability arises from insufficient interfacial adhesion at the metal-polymer boundary, manifesting as progressive delamination and impedance drift under cyclic mechanical loading. To address these challenges, we present a synergistic engineering strategy integrating three complementary approaches: geometric optimization of electrode array configurations, femtosecond laser-processed micro/nanostructured mechanical interlocks, and polymer matrix toughening through hexane-induced PDMS crosslinking modification. Finite element analysis and cyclic bending tests indicate that the optimized circular electrode array effectively distributes stress and alleviates stress concentration. Parametric Geometry Optimization enables active control of serpentine unit geometry, suppressing local stress and outperforming conventional designs under multi-axis loads.Furthermore, femtosecond laser processing creates periodic micro-nanostructures that form mechanical interlocks, significantly enhancing interfacial adhesion. Micro-Nano Interfacial Interlocking combines surface patterning with substrate modification to achieve robust adhesion, overcoming modulus mismatch. Additionally, hexane-modified PDMS improves polymer toughness, reinforcing the reliability of the interlocking structure. These innovations are integrated into a multi-scale design that synergizes geometric and material engineering, providing a comprehensive solution for long-term reliability of flexible implantable electrodes. This integrated approach increases Pt/PDMS interface bonding strength to 4.412 MPa, 9.74 times higher than that of the untreated samples, while reducing impedance fluctuations after cyclic bending (500 cycles, 80%) to 18.3%. These advancements collectively enable a new paradigm in durable flexible bioelectronics, where multiscale structural engineering synergistically enhances both mechanical robustness and functional reliability in chronic implantation scenarios.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"19 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947516","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}
Electrocatalytic co-reduction of carbon monoxide (CO) and nitric oxide (NO) to urea has tremendous potential as an alternative to traditional urea synthesis methods, simultaneously mitigating waste gas pollution. Herein, we report the synthesis of urea using single-atom catalysts (SACs) anchored on an α-borophene support. Density functional theory (DFT) computations reveal that anchoring SACs induces electron transfer to α-borophene, rendering the SACs and the adjacent B atoms to synergistically enhance the adsorption of NO reactants. Remarkably, the activated *NO couples with CO via a one-step N–C–N mechanism, with the anchored Ag atom exhibiting a low kinetic barrier of 0.58 eV. Furthermore, by computing the free energy changes of subsequent hydrogenation steps, Ag/α-borophene was identified as the most promising catalyst for urea production, demonstrating a record-low limiting potential (–0.20 V) attributable to its optimal interactions with NO reactants, as determined by its distinctive p- and d-band centers and charge distribution at active sites. Moreover, owing to its excellent suppression of competing side reactions, the Ag catalyst achieves high selectivity toward urea formation. In addition, a descriptor φ(η), incorporating the d-band center and charge transfer characteristics of the active metal for UL, was developed by employing the Sure Independence Screening and Sparsifying Operator (SISSO) method. Our findings offer a novel strategy for the rational design of next-generation catalysts by the co-catalysis between SACs and support.
{"title":"Insight into the critical role of synergy between the anchored single‑atoms and α‑borophene support for urea electrosynthesis from co-reduction of nitric oxide and carbon monoxide","authors":"Jiawei Dong , Daifei Ye , Zhenghaoyang Zhu , Xiaoyu Chen , Riguang Zhang , Jing Xu , Jingxiang Zhao","doi":"10.1016/j.apsusc.2026.165840","DOIUrl":"10.1016/j.apsusc.2026.165840","url":null,"abstract":"<div><div>Electrocatalytic co-reduction of carbon monoxide (CO) and nitric oxide (NO) to urea has tremendous potential as an alternative to traditional urea synthesis methods, simultaneously mitigating waste gas pollution. Herein, we report the synthesis of urea using single-atom catalysts (SACs) anchored on an α-borophene support. Density functional theory (DFT) computations reveal that anchoring SACs induces electron transfer to α-borophene, rendering the SACs and the adjacent B atoms to synergistically enhance the adsorption of NO reactants. Remarkably, the activated *NO couples with CO via a one-step N–C–N mechanism, with the anchored Ag atom exhibiting a low kinetic barrier of 0.58 eV. Furthermore, by computing the free energy changes of subsequent hydrogenation steps, Ag/α-borophene was identified as the most promising catalyst for urea production, demonstrating a record-low limiting potential (–0.20 V) attributable to its optimal interactions with NO reactants, as determined by its distinctive p- and d-band centers and charge distribution at active sites. Moreover, owing to its excellent suppression of competing side reactions, the Ag catalyst achieves high selectivity toward urea formation. In addition, a descriptor φ(η), incorporating the d-band center and charge transfer characteristics of the active metal for U<sub>L</sub>, was developed by employing the Sure Independence Screening and Sparsifying Operator (SISSO) method. Our findings offer a novel strategy for the rational design of next-generation catalysts by the co-catalysis between SACs and support.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165840"},"PeriodicalIF":6.9,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145938179","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}
In recent years, smart cellulosic nonwovens have emerged as a research hotspot due to their multifunctional integration capabilities. In this study, a multifunctional composite material (CNs-CaCO3-MoS2@TA) was fabricated through a stepwise fabrication process. First, tannic acid (TA) was employed to mediate the effective exfoliation of molybdenum disulfide (MoS2) into nanosheets (MoS2@TA). Subsequently, calcium carbonate (CaCO3) and the functionalized MoS2@TA nanosheets were successively integrated onto a cellulose nonwoven (CNs) substrate. Mechanical characterization revealed a significant enhancement in material strength compared to pure CNs, attributed to the synergistic effects between the interlayer-slip toughening mechanism of MoS2@TA and the rigid reinforcement provided by CaCO3. For photothermal conversion, the composite exhibited rapid heating characteristics under simulated sunlight, maintaining a surface temperature of 90 °C with excellent stability. This result benefits from the efficient combination of MoS2 broadband light absorption and CaCO3 light scattering effects. In addition, the CNs-CaCO3-MoS2@TA demonstrated 99.9% bactericidal efficiency against both E. coli and S. aureus through combined mechanisms including CaCO3-induced alkaline disruption, MoS2@TA-mediated photocatalytic ROS generation, and sharp nanosheet edge-induced physical membrane damages. These findings not only provide novel strategies for developing high-performance cellulose-based composites, but also open new avenues for smart nonwovens applications in medical and energy fields
{"title":"Synergistic effects of mineralized networks and functionalized molybdenum disulfide in a cellulose nonwoven composite for integrated mechanical, photothermal, and antibacterial performance","authors":"JinPu Li, Jiyuan Wen, Kuang Li, Meiling Chen, Shicun Jin, Huining Xiao","doi":"10.1016/j.apsusc.2026.165880","DOIUrl":"https://doi.org/10.1016/j.apsusc.2026.165880","url":null,"abstract":"In recent years, smart cellulosic nonwovens have emerged as a research hotspot due to their multifunctional integration capabilities. In this study, a multifunctional composite material (CNs-CaCO<ce:inf loc=\"post\">3</ce:inf>-MoS<ce:inf loc=\"post\">2</ce:inf>@TA) was fabricated through a stepwise fabrication process. First, tannic acid (TA) was employed to mediate the effective exfoliation of molybdenum disulfide (MoS<ce:inf loc=\"post\">2</ce:inf>) into nanosheets (MoS<ce:inf loc=\"post\">2</ce:inf>@TA). Subsequently, calcium carbonate (CaCO<ce:inf loc=\"post\">3</ce:inf>) and the functionalized MoS<ce:inf loc=\"post\">2</ce:inf>@TA nanosheets were successively integrated onto a cellulose nonwoven (CNs) substrate. Mechanical characterization revealed a significant enhancement in material strength compared to pure CNs, attributed to the synergistic effects between the interlayer-slip toughening mechanism of MoS<ce:inf loc=\"post\">2</ce:inf>@TA and the rigid reinforcement provided by CaCO<ce:inf loc=\"post\">3</ce:inf>. For photothermal conversion, the composite exhibited rapid heating characteristics under simulated sunlight, maintaining a surface temperature of 90 °C with excellent stability. This result benefits from the efficient combination of MoS<ce:inf loc=\"post\">2</ce:inf> broadband light absorption and CaCO<ce:inf loc=\"post\">3</ce:inf> light scattering effects. In addition, the CNs-CaCO<ce:inf loc=\"post\">3</ce:inf>-MoS<ce:inf loc=\"post\">2</ce:inf>@TA demonstrated 99.9% bactericidal efficiency against both <ce:italic>E. coli</ce:italic> and <ce:italic>S. aureus</ce:italic> through combined mechanisms including CaCO<ce:inf loc=\"post\">3</ce:inf>-induced alkaline disruption, MoS<ce:inf loc=\"post\">2</ce:inf>@TA-mediated photocatalytic ROS generation, and sharp nanosheet edge-induced physical membrane damages. These findings not only provide novel strategies for developing high-performance cellulose-based composites, but also open new avenues for smart nonwovens applications in medical and energy fields","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"21 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956548","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}
Pub Date : 2026-01-10DOI: 10.1016/j.apsusc.2026.165842
Dorien E. Carpenter , Zahra Nasiri , Nithesh R. Palagiri , Kamron L. Strickland , Sumner B. Harris , David B. Geohegan , Renato P. Camata
Mesoporous films of the metal chalcogenide -FeSe were grown on MgO substrates by KrF pulsed laser deposition (PLD) in an argon background. At 100 mTorr, gated intensified charge-coupled device imaging and ion probe measurements showed that the plasma plume responsible for crystal growth initially comprised three components, with distinct expansion velocities. Plume interactions with the substrate heater and ablation target gave rise to complex dynamics, including collisions between the charged leading edge—rebounding between the substrate and the target—and slower-moving species in the plume interior. Film growth was dominated by species with kinetic energies 0.5 eV/atom. X-ray reflectivity revealed that films grown in this environment—with a substrate temperature of 350 C, a laser fluence of 1.0 J cm−2, and a 7.5 mm spot area—formed a porous framework with 15% porosity. Atomic force microscopy showed surface features that suggest pore sizes below 100 nm. X-ray diffraction indicated that the porous films were epitaxial with respect to the substrate and likely grew by oriented-attachment of gas-phase molecular clusters or very small nanoparticles, in contrast to the conventional epitaxy of vacuum films from atomic constituents. The in-plane orientation of the mesoporous films was -FeSe [100][110] MgO, attributed to the soft landing of pre-formed crystallites on the MgO substrates, where protruding Se rows of -FeSe aligned with corrugations of the MgO surface. This work implies that growth of candidate electrocatalyst materials by PLD in inert gas background may allow mesoporous frameworks with a single crystallographic orientation that expose specific crystal facets for electrochemical reactions and active site engineering.
Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).
{"title":"Pulsed laser synthesis of mesoporous metal chalcogenide thin films","authors":"Dorien E. Carpenter , Zahra Nasiri , Nithesh R. Palagiri , Kamron L. Strickland , Sumner B. Harris , David B. Geohegan , Renato P. Camata","doi":"10.1016/j.apsusc.2026.165842","DOIUrl":"10.1016/j.apsusc.2026.165842","url":null,"abstract":"<div><div>Mesoporous films of the metal chalcogenide <span><math><mi>β</mi></math></span>-FeSe were grown on MgO substrates by KrF pulsed laser deposition (PLD) in an argon background. At 100 mTorr, gated intensified charge-coupled device imaging and ion probe measurements showed that the plasma plume responsible for crystal growth initially comprised three components, with distinct expansion velocities. Plume interactions with the substrate heater and ablation target gave rise to complex dynamics, including collisions between the charged leading edge—rebounding between the substrate and the target—and slower-moving species in the plume interior. Film growth was dominated by species with kinetic energies <span><math><mo>≤</mo></math></span>0.5 eV/atom. X-ray reflectivity revealed that films grown in this environment—with a substrate temperature of 350 <span><math><mo>°</mo></math></span>C, a laser fluence of 1.0 J cm<sup>−2</sup>, and a 7.5 mm<span><math><msup><mrow></mrow><mrow><mn>2</mn></mrow></msup></math></span> spot area—formed a porous framework with 15% porosity. Atomic force microscopy showed surface features that suggest pore sizes below 100 nm. X-ray diffraction indicated that the porous films were epitaxial with respect to the substrate and likely grew by oriented-attachment of gas-phase molecular clusters or very small nanoparticles, in contrast to the conventional epitaxy of vacuum films from atomic constituents. The in-plane orientation of the mesoporous films was <span><math><mi>β</mi></math></span>-FeSe [100]<span><math><mo>∥</mo></math></span>[110] MgO, attributed to the soft landing of pre-formed crystallites on the MgO substrates, where protruding Se rows of <span><math><mi>β</mi></math></span>-FeSe aligned with corrugations of the MgO surface. This work implies that growth of candidate electrocatalyst materials by PLD in inert gas background may allow mesoporous frameworks with a single crystallographic orientation that expose specific crystal facets for electrochemical reactions and active site engineering.</div><div>Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (<span><span>http://energy.gov/downloads/doe-public-access-plan</span><svg><path></path></svg></span>).</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"726 ","pages":"Article 165842"},"PeriodicalIF":6.9,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956581","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}
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