Jiefu Yang, Ruijia Sun, Xuan Bao, Juanjuan Liu, Jun Wen Ng, Bijun Tang, Zheng Liu
Two-dimensional (2D) materials have emerged as promising candidates for gas sensing applications due to their exceptional electrical, structural, and chemical properties, which enable high sensitivity and rapid response to gas molecules. However, despite their potential, 2D material-based gas sensors face a significant challenge in achieving adequate selectivity, as many sensors respond similarly to multiple gases, leading to cross-sensitivity and inaccurate detection. This review provides a comprehensive overview of the recent advancements for improving the selectivity of 2D gas sensors. It explores material modification strategies, such as functionalizing the sensing components and tuning adsorption dynamics, to enhance selective gas interactions. Engineering approaches, including field-effect modulation and sensor array design, are also discussed as effective methods to fine-tune sensor performance. Additionally, the integration of machine learning (ML) algorithms is highlighted for their potential to differentiate among multiple analytes. Prospects for further improving selectivity through material optimization, sensor calibration, and drift compensation are explored, along with the incorporation of smart sensing systems into the Internet of Things (IoT). This review outlines key objectives and strategies that pave the way for next-generation gas sensors with enhanced selectivity, reliability, and versatility, poised to impact a wide range of applications from environmental monitoring to industrial safety.
{"title":"Enhancing Selectivity of Two-Dimensional Materials-Based Gas Sensors","authors":"Jiefu Yang, Ruijia Sun, Xuan Bao, Juanjuan Liu, Jun Wen Ng, Bijun Tang, Zheng Liu","doi":"10.1002/adfm.202420393","DOIUrl":"https://doi.org/10.1002/adfm.202420393","url":null,"abstract":"Two-dimensional (2D) materials have emerged as promising candidates for gas sensing applications due to their exceptional electrical, structural, and chemical properties, which enable high sensitivity and rapid response to gas molecules. However, despite their potential, 2D material-based gas sensors face a significant challenge in achieving adequate selectivity, as many sensors respond similarly to multiple gases, leading to cross-sensitivity and inaccurate detection. This review provides a comprehensive overview of the recent advancements for improving the selectivity of 2D gas sensors. It explores material modification strategies, such as functionalizing the sensing components and tuning adsorption dynamics, to enhance selective gas interactions. Engineering approaches, including field-effect modulation and sensor array design, are also discussed as effective methods to fine-tune sensor performance. Additionally, the integration of machine learning (ML) algorithms is highlighted for their potential to differentiate among multiple analytes. Prospects for further improving selectivity through material optimization, sensor calibration, and drift compensation are explored, along with the incorporation of smart sensing systems into the Internet of Things (IoT). This review outlines key objectives and strategies that pave the way for next-generation gas sensors with enhanced selectivity, reliability, and versatility, poised to impact a wide range of applications from environmental monitoring to industrial safety.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"16 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Microwave absorption materials play a key role in various fields, including military stealth, human safety protection, and so on. Construction of 2D mesoporous heterostructures is an attractive approach to enhance wave-absorbing ability, while it is still a great challenge. Herein, 2D mesoporous carbon-MXene-carbon heterostructures (MCMCH) with channels parallel to surface are successfully prepared via a monolayer interfacial assembly strategy. Through the precise adjustment and polymerization, cylindrical micelles orderly monolayered assemble on both surfaces of 2D MXene nanosheets, resulting in 2D switch-like polydopamine-MXene-polydopamine nanosheets, and 2D MCMCH are finally generated by further calcination. Due to the excellent dielectric polarization relaxation and conductive loss, MCMCH achieves the strongest reflection loss of −54.2 dB at a thickness of only 1.5 mm. The presence of mesochannels not only introduces air with a low permittivity for optimal impedance matching, but also further extends the attenuation path of the incident electromagnetic wave. The maximum radar cross-section reduction of 26.9 dB m2 is achieved for the MCMCH compared to the perfect electric conductor. This work provides a reference for surface engineering based on 2D mesoporous heterostructures to enhance the microwave absorption performance.
{"title":"Monolayer Interfacial Assembly toward Two-Dimensional Mesoporous Heterostructure for Boosting Wave Absorption","authors":"Zelin Zhang, Aibing Chen, Xiao Li, Ruonan Li, Haowei Zhou, Zhongming Liu, Xinyue Zhang, Xudong Jing, Zhongxue Lin, Di Zhou, Biao Kong, Lei Xie","doi":"10.1002/adfm.202420702","DOIUrl":"https://doi.org/10.1002/adfm.202420702","url":null,"abstract":"Microwave absorption materials play a key role in various fields, including military stealth, human safety protection, and so on. Construction of 2D mesoporous heterostructures is an attractive approach to enhance wave-absorbing ability, while it is still a great challenge. Herein, 2D mesoporous carbon-MXene-carbon heterostructures (MCMCH) with channels parallel to surface are successfully prepared via a monolayer interfacial assembly strategy. Through the precise adjustment and polymerization, cylindrical micelles orderly monolayered assemble on both surfaces of 2D MXene nanosheets, resulting in 2D switch-like polydopamine-MXene-polydopamine nanosheets, and 2D MCMCH are finally generated by further calcination. Due to the excellent dielectric polarization relaxation and conductive loss, MCMCH achieves the strongest reflection loss of −54.2 dB at a thickness of only 1.5 mm. The presence of mesochannels not only introduces air with a low permittivity for optimal impedance matching, but also further extends the attenuation path of the incident electromagnetic wave. The maximum radar cross-section reduction of 26.9 dB m<sup>2</sup> is achieved for the MCMCH compared to the perfect electric conductor. This work provides a reference for surface engineering based on 2D mesoporous heterostructures to enhance the microwave absorption performance.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"27 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968642","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Luminescent solar concentrators (LSCs) can convert sunlight to clean energy by serving as large-area collectors of sunlight. Benefiting from their large-area, semi-transparency, and lightweight characteristics, LSCs have gained a great of attention. However, their optical efficiency is limited by the low quantum yield (QY) and small Stokes shift of conventional photoluminescent materials. Carbon quantum dots (C-dots) are promising alternatives, yet achieving both high QY and large Stokes shift has proven challenging. Here, a simple, controllable vacuum heating method is introduced to synthesize highly efficient C-dots using a citric acid-urea-cyanuric acid-CaCl2 system. The cyanuric acid-capped C-dots exhibit outstanding properties, including a QY of 94.3% in solution and 100% in a polymer matrix, a large Stokes shift of 0.64 eV, and exceptional photostability, making them ideal for LSC applications. Ultrafast transient absorption spectroscopy provides insights into their exciton dynamics. An LSC (25 cm2) based on these C-dots achieves an optical efficiency of 13.82% ± 0.30%, while its attached photovoltaic cell attains a power conversion efficiency of 4.82% ± 0.10% under natural sunlight (80 mW cm−2), marking the highest performance reported for C-dot-based LSCs. These results highlight the potential of cyanuric acid-capped C-dots for advanced solid-state lighting and energy conversion technologies.
发光太阳能聚光器（LSCs）可作为大面积的太阳光收集器，将太阳光转化为清洁能源。由于具有大面积、半透明和重量轻的特点，发光太阳能聚光器受到了广泛关注。然而，传统光致发光材料的量子产率（QY）低、斯托克斯位移小，限制了它们的光学效率。碳量子点（C-dots）是一种很有前景的替代材料，但要同时实现高量子产率和大斯托克斯位移却具有挑战性。本文介绍了一种简单、可控的真空加热方法，利用柠檬酸-尿素-氰尿酸-CaCl2 体系合成高效的碳量子点。氰尿酸封端的 C 点表现出卓越的性能，包括溶液中 94.3% 的 QY 值和聚合物基质中 100% 的 QY 值、0.64 eV 的大斯托克斯位移以及优异的光稳定性，使其成为 LSC 应用的理想选择。超快瞬态吸收光谱可以深入了解它们的激子动力学。基于这些 C 点的 LSC（25 cm2）的光学效率达到了 13.82% ± 0.30%，而其附带的光伏电池在自然阳光（80 mW cm-2）下的功率转换效率为 4.82% ± 0.10%，这是目前已报道的基于 C 点的 LSC 的最高性能。这些结果凸显了三聚氰酸封端的 C 点在先进固态照明和能源转换技术方面的潜力。
{"title":"Highly Efficient Luminescent Solar Concentrators Based on Capped Carbon Quantum Dots with Unity Quantum Yield","authors":"Lihua Wang, Xiaohan Wang, Haiguang Zhao","doi":"10.1002/adfm.202423422","DOIUrl":"https://doi.org/10.1002/adfm.202423422","url":null,"abstract":"Luminescent solar concentrators (LSCs) can convert sunlight to clean energy by serving as large-area collectors of sunlight. Benefiting from their large-area, semi-transparency, and lightweight characteristics, LSCs have gained a great of attention. However, their optical efficiency is limited by the low quantum yield (QY) and small Stokes shift of conventional photoluminescent materials. Carbon quantum dots (C-dots) are promising alternatives, yet achieving both high QY and large Stokes shift has proven challenging. Here, a simple, controllable vacuum heating method is introduced to synthesize highly efficient C-dots using a citric acid-urea-cyanuric acid-CaCl<sub>2</sub> system. The cyanuric acid-capped C-dots exhibit outstanding properties, including a QY of 94.3% in solution and 100% in a polymer matrix, a large Stokes shift of 0.64 eV, and exceptional photostability, making them ideal for LSC applications. Ultrafast transient absorption spectroscopy provides insights into their exciton dynamics. An LSC (25 cm<sup>2</sup>) based on these C-dots achieves an optical efficiency of 13.82% ± 0.30%, while its attached photovoltaic cell attains a power conversion efficiency of 4.82% ± 0.10% under natural sunlight (80 mW cm<sup>−2</sup>), marking the highest performance reported for C-dot-based LSCs. These results highlight the potential of cyanuric acid-capped C-dots for advanced solid-state lighting and energy conversion technologies.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"16 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968645","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Silicon-carbon composites (Si/C) with multistage structures enable structural integrity during cycling. However, the lack of controllable structure preparation on a large scale hinders the stability improvement in practical applications. Herein, a new strategy is proposed to synthesize kilogram-scale Si/C (PySi/C) featuring a dual-model carbon structure in one step. The controllable combination of an onion-like carbon coating on the Si surface with independent pyrolytic carbon is accomplished through the precise adjustment of the pyrolysis temperature. The dual-model carbon formation mechanism is unraveled, detailing the cooperative coupling of the nucleation laws of carbon compositions as well as the changes trends in morphology and crystallinity. This density functional theory and finite element analysis highlight the dual-model structure's essential contribution to the electrochemical behavior and structural stability. As expected, PySi/Cs anodes deliver stable cycling performance with retention of 91.5% after 800 cycles at 2 A g−1. Its comprehensive electrochemical performance surpasses that of the state-of-the-art kilogram-scale Si-based anode reported. Moreover, the assembled pouch cell exhibits actual competitiveness, showing a capacity of 1.97 Ah and a retention of 88.9% after 300 cycles at 1 C. This work provides valuable design concepts to further advance the development of Si/C anodes.
{"title":"Orchestrating a Controllable Engineering of Dual-Model Carbon Structure in Si/C Anodes","authors":"Jiapeng Zhang, Renlu Yuan, Dengke Wang, Jiangchuan Li, Xue Yao, Lixin Chen, Xiaotian Li, Zhijie Jiang, Haiyan Liu, Yu Hou, Ang Li, Xiaohong Chen, Zhiwen Chen, Chandra Veer Singh, Huaihe Song","doi":"10.1002/adfm.202423700","DOIUrl":"https://doi.org/10.1002/adfm.202423700","url":null,"abstract":"Silicon-carbon composites (Si/C) with multistage structures enable structural integrity during cycling. However, the lack of controllable structure preparation on a large scale hinders the stability improvement in practical applications. Herein, a new strategy is proposed to synthesize kilogram-scale Si/C (PySi/C) featuring a dual-model carbon structure in one step. The controllable combination of an onion-like carbon coating on the Si surface with independent pyrolytic carbon is accomplished through the precise adjustment of the pyrolysis temperature. The dual-model carbon formation mechanism is unraveled, detailing the cooperative coupling of the nucleation laws of carbon compositions as well as the changes trends in morphology and crystallinity. This density functional theory and finite element analysis highlight the dual-model structure's essential contribution to the electrochemical behavior and structural stability. As expected, PySi/Cs anodes deliver stable cycling performance with retention of 91.5% after 800 cycles at 2 A g<sup>−1</sup>. Its comprehensive electrochemical performance surpasses that of the state-of-the-art kilogram-scale Si-based anode reported. Moreover, the assembled pouch cell exhibits actual competitiveness, showing a capacity of 1.97 Ah and a retention of 88.9% after 300 cycles at 1 C. This work provides valuable design concepts to further advance the development of Si/C anodes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Although high-entropy materials have garnered extensive attention due to their substantially enhanced performance, their formation generally demands prolonged high-temperature synthetic processes. Moreover, research on entropy-stabilized halide perovskite (ESHP) semiconductor colloidal nanocrystals (NCs) is scarce. Herein, a highly efficient and rapid room temperature (RT) entropy-stabilized approach in air is proposed, involving the concurrent incorporation of multi-metal cations for the synthesis of high-quality all-inorganic ESHP NCs with near-unity quantum yield and excellent colloidal stability. Remarkably, even after 8 months of aging in air, the ESHP NCs exhibited superior emission characteristics with a single-exponential decay and maintained the initial NC monodispersity. Density functional theory calculations further demonstrated that the outstanding performance of ESHP NCs originated from the diminished crystal defects and a more robust octahedral structure. Significantly, this RT entropy-driven synthesis can be extended to metal halide semiconductor NCs with diverse composition systems. The findings inspire new perspectives for entropy-stabilized, high-performance metal halide perovskite NCs toward versatile applications.
{"title":"Rapid Room Temperature Entropy-Stabilized Synthesis Enabling Super-Stable Metal Halide Perovskite Semiconductor Colloidal Nanocrystals","authors":"Louwen Zhang, Yibo Chen, Zhimiao Zheng, Yuan Zhou, Chen Li, Guang Li, Bin Ren, Zhongqiang Hu, Hai Zhou, Fuqiang Ren, Weijun Ke, Guojia Fang","doi":"10.1002/adfm.202423450","DOIUrl":"https://doi.org/10.1002/adfm.202423450","url":null,"abstract":"Although high-entropy materials have garnered extensive attention due to their substantially enhanced performance, their formation generally demands prolonged high-temperature synthetic processes. Moreover, research on entropy-stabilized halide perovskite (ESHP) semiconductor colloidal nanocrystals (NCs) is scarce. Herein, a highly efficient and rapid room temperature (RT) entropy-stabilized approach in air is proposed, involving the concurrent incorporation of multi-metal cations for the synthesis of high-quality all-inorganic ESHP NCs with near-unity quantum yield and excellent colloidal stability. Remarkably, even after 8 months of aging in air, the ESHP NCs exhibited superior emission characteristics with a single-exponential decay and maintained the initial NC monodispersity. Density functional theory calculations further demonstrated that the outstanding performance of ESHP NCs originated from the diminished crystal defects and a more robust octahedral structure. Significantly, this RT entropy-driven synthesis can be extended to metal halide semiconductor NCs with diverse composition systems. The findings inspire new perspectives for entropy-stabilized, high-performance metal halide perovskite NCs toward versatile applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"49 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968648","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pei Lyu, Wenwen Shi, Yuemei Liu, Rui Ding, Jun Hu, Bin Shang, Heng Pan, Jie Ren, Xin Liu, Weilin Xu
Passive deicing technologies achieved by dynamic superhydrophobic surfaces and slippery substances contribute to widely used anti-icing. However, the constant status of microstructures cannot cater to the changing environment, meanwhile, the energy barrier needs to be improved. Here, a dynamic superhydrophobic standing-fiber surface with a three-level energy barrier is fabricated by electrical flocking technology, which directly utilizes the wind field to assist anti-icing. The standing-fiber surface has low ice adhesion of 2.7 kPa, a high water contact angle of 171.1°, and a long icing delay time of 859 s under −30 °C. The superhydrophobicity contributes to excellent water repellency with a droplet retracting and bouncing distance of 3.53 and 3.75 mm. In the wind field at 9 ms−1, the inclined standing-fiber surface theoretically accelerates the motion of the water droplet by 1.5 times compared with the lying-fiber surface. The difference in thermal conductivity between the front and back sides of the standing-fiber surface makes it an ideal candidate for designing anti-icing, deicing, and thermal insulation clothes.
{"title":"Adaptable, Dynamic, and Superhydrophobic Standing-Fiber Surface with Muti-Level Energy Barrier for Anti-Icing","authors":"Pei Lyu, Wenwen Shi, Yuemei Liu, Rui Ding, Jun Hu, Bin Shang, Heng Pan, Jie Ren, Xin Liu, Weilin Xu","doi":"10.1002/adfm.202421174","DOIUrl":"https://doi.org/10.1002/adfm.202421174","url":null,"abstract":"Passive deicing technologies achieved by dynamic superhydrophobic surfaces and slippery substances contribute to widely used anti-icing. However, the constant status of microstructures cannot cater to the changing environment, meanwhile, the energy barrier needs to be improved. Here, a dynamic superhydrophobic standing-fiber surface with a three-level energy barrier is fabricated by electrical flocking technology, which directly utilizes the wind field to assist anti-icing. The standing-fiber surface has low ice adhesion of 2.7 kPa, a high water contact angle of 171.1°, and a long icing delay time of 859 s under −30 °C. The superhydrophobicity contributes to excellent water repellency with a droplet retracting and bouncing distance of 3.53 and 3.75 mm. In the wind field at 9 ms<sup>−1</sup>, the inclined standing-fiber surface theoretically accelerates the motion of the water droplet by 1.5 times compared with the lying-fiber surface. The difference in thermal conductivity between the front and back sides of the standing-fiber surface makes it an ideal candidate for designing anti-icing, deicing, and thermal insulation clothes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"51 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jianglei Zhang, Weijun Li, Yifan Yang, Zigao Tang, Haotong Wei, Junhu Zhang, Bai Yang
Given the promising application prospects of underwater X-ray detection technology, traditional perovskite materials, despite their outstanding performance in X-ray detection, are significantly constrained by their inherent susceptibility to hydrolysis, hindering their effective utilization in underwater environments. To date, most efforts are devoted to evaluating these materials' performance under atmospheric conditions, with a limited exploration into their adaptability in underwater settings. In this study, the successful fabrication of thick perovskite single-crystal arrays with a thickness of 400 µm and their integration into a stable underwater X-ray detector array is demonstrated. The single-crystal arrays exhibit remarkable uniformity in both alignment and dimensions, thereby contributing to improved detection homogeneity and enhanced underwater imaging capabilities. The detector arrays exhibit exceptional X-ray detection performance, characterized by a high sensitivity of 155,020 µC·Gy−1·cm−2 at 5 V bias and a low detection limit of 52 nGy·s−1, which represents a significant advancement in the frontier of perovskite-based materials for underwater X-ray detection. After continuous submersion in water for over 60 days, the detector array maintains its initial X-ray detection performance, proving its stable adaptability to the underwater environment.
鉴于水下 X 射线探测技术具有广阔的应用前景，传统的过氧化物晶体材料尽管在 X 射线探测方面表现出色，但却因其固有的易水解性而受到很大限制，阻碍了它们在水下环境中的有效利用。迄今为止，大多数研究都致力于评估这些材料在大气条件下的性能，而对其在水下环境中的适应性的探索还很有限。在本研究中，成功地制造出厚度为 400 微米的厚包晶单晶阵列，并将其集成到稳定的水下 X 射线探测器阵列中。单晶阵列在排列和尺寸上都表现出显著的一致性，从而有助于提高探测均匀性和增强水下成像能力。探测器阵列具有优异的 X 射线探测性能，在 5 V 偏压条件下灵敏度高达 155,020 µC-Gy-1-cm-2，探测极限低至 52 nGy-s-1，这标志着在水下 X 射线探测的透辉石基材料前沿领域取得了重大进展。在水中连续浸泡 60 多天后，探测器阵列仍能保持最初的 X 射线探测性能，证明了其对水下环境的稳定适应性。
{"title":"Integrated Underwater X-Ray Detector Arrays Fabricated by Perovskite Single-Crystal Arrays","authors":"Jianglei Zhang, Weijun Li, Yifan Yang, Zigao Tang, Haotong Wei, Junhu Zhang, Bai Yang","doi":"10.1002/adfm.202422003","DOIUrl":"https://doi.org/10.1002/adfm.202422003","url":null,"abstract":"Given the promising application prospects of underwater X-ray detection technology, traditional perovskite materials, despite their outstanding performance in X-ray detection, are significantly constrained by their inherent susceptibility to hydrolysis, hindering their effective utilization in underwater environments. To date, most efforts are devoted to evaluating these materials' performance under atmospheric conditions, with a limited exploration into their adaptability in underwater settings. In this study, the successful fabrication of thick perovskite single-crystal arrays with a thickness of 400 µm and their integration into a stable underwater X-ray detector array is demonstrated. The single-crystal arrays exhibit remarkable uniformity in both alignment and dimensions, thereby contributing to improved detection homogeneity and enhanced underwater imaging capabilities. The detector arrays exhibit exceptional X-ray detection performance, characterized by a high sensitivity of 155,020 µC·Gy<sup>−1</sup>·cm<sup>−2</sup> at 5 V bias and a low detection limit of 52 nGy·s<sup>−1</sup>, which represents a significant advancement in the frontier of perovskite-based materials for underwater X-ray detection. After continuous submersion in water for over 60 days, the detector array maintains its initial X-ray detection performance, proving its stable adaptability to the underwater environment.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"43 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968646","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Liyang Lv, Hao Tan, Yuying Liu, Na Li, Qianqian Ji, Yuan Kong, Huijuan Wang, Mei Sun, Minghui Fan, Chao Wang, Wensheng Yan
The electrochemical transformation of nitrate (NO3−) into ammonia (NH3) holds significant promise to addresses nitration contamination and offers a sustainable alternative to the Haber–Bosch process. However, the sluggish kinetics hinders its large‐scale application. Herein, a Cu‐doped SrRuO3 synergetic tandem catalyst is designed and synthesized, which demonstrates exceptional performance in converting NO3− to NH3. Specifically, this catalyst achieves a maximum Faradaic efficiency of 95.4% for ammonia production, along with a high yield rate of 7196 µg h−1 mgcat.−1. A series of detailed characterizations reveals that the doped Cu ions modify the local electronic environment of Ru 4d eg orbital in SrRuO3, thereby facilitating highly efficient electron transfer processes. In situ delta X‐ray absorption near‐edge structure (ΔXANES), synchrotron radiation‐based Fourier transform infrared (SR‐FTIR) and Raman spectroscopy identified the *NO2− generated on the Cu active sites is subsequently hydrogenated on the Ru sites. Combined with theoretical studies, it is confirmed that the tandem catalyst significantly reduces the energy barriers of the rate‐determining step (*NO to *NOH), thereby enhancing the efficiency of ammonia synthesis. This work not only offers fundamental insights into the mechanisms of cation substitution on regulating the eg orbital of perovskite catalysts, but also provides a promising avenue for the electro‐synthesis of ammonia.
{"title":"Cu‐Ru Bicenter Synergistically Triggers Tandem Catalytic Effect for Electroreduction of Nitrate to Ammonium","authors":"Liyang Lv, Hao Tan, Yuying Liu, Na Li, Qianqian Ji, Yuan Kong, Huijuan Wang, Mei Sun, Minghui Fan, Chao Wang, Wensheng Yan","doi":"10.1002/adfm.202423612","DOIUrl":"https://doi.org/10.1002/adfm.202423612","url":null,"abstract":"The electrochemical transformation of nitrate (NO<jats:sub>3</jats:sub><jats:sup>−</jats:sup>) into ammonia (NH<jats:sub>3</jats:sub>) holds significant promise to addresses nitration contamination and offers a sustainable alternative to the Haber–Bosch process. However, the sluggish kinetics hinders its large‐scale application. Herein, a Cu‐doped SrRuO<jats:sub>3</jats:sub> synergetic tandem catalyst is designed and synthesized, which demonstrates exceptional performance in converting NO<jats:sub>3</jats:sub><jats:sup>−</jats:sup> to NH<jats:sub>3</jats:sub>. Specifically, this catalyst achieves a maximum Faradaic efficiency of 95.4% for ammonia production, along with a high yield rate of 7196 µg h<jats:sup>−1</jats:sup> mg<jats:sub>cat.</jats:sub><jats:sup>−1</jats:sup>. A series of detailed characterizations reveals that the doped Cu ions modify the local electronic environment of Ru 4<jats:italic>d e</jats:italic><jats:sub>g</jats:sub> orbital in SrRuO<jats:sub>3</jats:sub>, thereby facilitating highly efficient electron transfer processes. In situ delta X‐ray absorption near‐edge structure (ΔXANES), synchrotron radiation‐based Fourier transform infrared (SR‐FTIR) and Raman spectroscopy identified the <jats:sup>*</jats:sup>NO<jats:sub>2</jats:sub><jats:sup>−</jats:sup> generated on the Cu active sites is subsequently hydrogenated on the Ru sites. Combined with theoretical studies, it is confirmed that the tandem catalyst significantly reduces the energy barriers of the rate‐determining step (<jats:sup>*</jats:sup>NO to <jats:sup>*</jats:sup>NOH), thereby enhancing the efficiency of ammonia synthesis. This work not only offers fundamental insights into the mechanisms of cation substitution on regulating the <jats:italic>e<jats:sub>g</jats:sub></jats:italic> orbital of perovskite catalysts, but also provides a promising avenue for the electro‐synthesis of ammonia.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"48 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961621","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Developing overall water splitting non‐noble metal electrocatalysts achieving long‐term stability with high activity at industrial‐grade current density remains challenging. Herein, a self‐reconstruction strategy of Co9S8‐Ni3S2/NCF is employed to fabricate NixCo3‐xO4‐Ov‐ in which partial Co is replaced by Ni in the structure. The reconstructed NixCo3‐xO4‐Ov can enhance the adsorbing ability of leached from the initial phase compared with Co spinel, achieving exceeding 1000‐h oxygen evolution reaction (OER) and 600‐h overall water splitting stability at 1000 mA cm−2 with excellent activity. In situ Raman and X‐ray photoelectron spectroscopy (XPS) results indicate that partial substitution of Ni for Co atoms enhances the adsorption capacity on the reconstructed NixCo3‐xO4‐Ov, facilitating the formation of high‐density Co3+ active sites on (400) that expedited interfacial electron transfer at high current densities. Density functional theory (DFT) calculations reveal that the adsorption of leached stabilizes surface oxygen vacancies and optimizes the adsorption energy of intermediates, thereby improving both stability and catalytic performance. The findings provide new insights into overcoming the activity‐stability trade‐off and contribute to the strategy for the design of electrocatalysts for long‐term water splitting at industrial‐grade current densities.
{"title":"Self‐Reconstructed Spinel with Enhanced SO42− Adsorption and Highly Exposed Co3+ From Heterostructure Boosts Activity and Stability at High Current Density for Overall Water Splitting","authors":"Hongye Yang, Fafa Chen, Xusheng Wang, Jinjie Qian, Jiajun Wang, Jiahao Li, Chang Lv, Lan Li, Sateesh Bandaru, Junkuo Gao","doi":"10.1002/adfm.202419978","DOIUrl":"https://doi.org/10.1002/adfm.202419978","url":null,"abstract":"Developing overall water splitting non‐noble metal electrocatalysts achieving long‐term stability with high activity at industrial‐grade current density remains challenging. Herein, a self‐reconstruction strategy of Co<jats:sub>9</jats:sub>S<jats:sub>8</jats:sub>‐Ni<jats:sub>3</jats:sub>S<jats:sub>2</jats:sub>/NCF is employed to fabricate Ni<jats:sub>x</jats:sub>Co<jats:sub>3‐x</jats:sub>O<jats:sub>4</jats:sub>‐Ov‐ in which partial Co is replaced by Ni in the structure. The reconstructed Ni<jats:sub>x</jats:sub>Co<jats:sub>3‐x</jats:sub>O<jats:sub>4</jats:sub>‐Ov can enhance the adsorbing ability of leached from the initial phase compared with Co spinel, achieving exceeding 1000‐h oxygen evolution reaction (OER) and 600‐h overall water splitting stability at 1000 mA cm<jats:sup>−2</jats:sup> with excellent activity. In situ Raman and X‐ray photoelectron spectroscopy (XPS) results indicate that partial substitution of Ni for Co atoms enhances the adsorption capacity on the reconstructed Ni<jats:sub>x</jats:sub>Co<jats:sub>3‐x</jats:sub>O<jats:sub>4</jats:sub>‐Ov, facilitating the formation of high‐density Co<jats:sup>3+</jats:sup> active sites on (400) that expedited interfacial electron transfer at high current densities. Density functional theory (DFT) calculations reveal that the adsorption of leached stabilizes surface oxygen vacancies and optimizes the adsorption energy of intermediates, thereby improving both stability and catalytic performance. The findings provide new insights into overcoming the activity‐stability trade‐off and contribute to the strategy for the design of electrocatalysts for long‐term water splitting at industrial‐grade current densities.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"6 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xu Wei, Hao Xie, Can Liu, Yan Li, Kai Sun, Baoyu Qi, Xiangyun Guo, Zhaofeng Liu, Xinlin Huang, Chuanrui Sun, Jian Wang, Yili Zhang, Lei Fan, Liguo Zhu
Bone fractures, especially large and complex defects, continue to pose significant challenges in the medical field. Current treatments often rely on autografts or allografts for structural support, which can lead to problems such as reduced bioactivity, infection risks, and potential pathogen transmission. Nature herbal medicine (NHM), including herbs and herbal extracts, offers a promising alternative by effectively modulating inflammatory responses, enhancing osteoblast function, and inhibiting bone resorption, thereby facilitating fracture repair. However, traditional drug delivery methods for NHM encounter challenges such as potential drug interactions, poor tissue distribution, and reduced patient compliance. Biomaterials, engineered to interact with biological systems, play essential roles in tissue repair, mechanical support, and drug delivery. When used as drug carriers, biomaterials can be combined with NHM to form stable drug delivery systems that further promote bone regeneration. Here the applications of biomaterials are reviewed, such as hydrogels, extracellular vesicles, and bone cement, in conjunction with NHM for regulating bone homeostasis and fracture repair, aiming to provide valuable insights and guidance for future research and therapeutic strategies.
{"title":"Nature Herbal Medicine‐ Tissue Engineering Strategies for Regulate Cell Homeostasis in Bone Regeneration","authors":"Xu Wei, Hao Xie, Can Liu, Yan Li, Kai Sun, Baoyu Qi, Xiangyun Guo, Zhaofeng Liu, Xinlin Huang, Chuanrui Sun, Jian Wang, Yili Zhang, Lei Fan, Liguo Zhu","doi":"10.1002/adfm.202417810","DOIUrl":"https://doi.org/10.1002/adfm.202417810","url":null,"abstract":"Bone fractures, especially large and complex defects, continue to pose significant challenges in the medical field. Current treatments often rely on autografts or allografts for structural support, which can lead to problems such as reduced bioactivity, infection risks, and potential pathogen transmission. Nature herbal medicine (NHM), including herbs and herbal extracts, offers a promising alternative by effectively modulating inflammatory responses, enhancing osteoblast function, and inhibiting bone resorption, thereby facilitating fracture repair. However, traditional drug delivery methods for NHM encounter challenges such as potential drug interactions, poor tissue distribution, and reduced patient compliance. Biomaterials, engineered to interact with biological systems, play essential roles in tissue repair, mechanical support, and drug delivery. When used as drug carriers, biomaterials can be combined with NHM to form stable drug delivery systems that further promote bone regeneration. Here the applications of biomaterials are reviewed, such as hydrogels, extracellular vesicles, and bone cement, in conjunction with NHM for regulating bone homeostasis and fracture repair, aiming to provide valuable insights and guidance for future research and therapeutic strategies.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"40 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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