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Biomimetic Intrafibrillar Mineralization of Hierarchically Structured Amyloid-Like Fibrils
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202416824
Shuting Miao, Jing Guo, Yuexin Zhang, Peisheng Liu, Xiaojie Chen, Qian Han, Yingbo Wang, Kun Xuan, Peng Yang, Fei Tao
Intrafibrillar mineralization is essential not only as a fundamental process in forming biological hard tissues but also as a foundation for developing advanced composite fibril-based materials for innovative applications. Traditionally, only natural collagen fibrils have been shown to enable intrafibrillar mineralization, presenting a challenge in designing ordered hierarchical fibrils from common protein aggregation that exhibit similar high intrafibrillar mineralization activity. In this study, a mechanically directed two-step transformation method is developed that converts phase-transitioned protein nanofilms into crystalline, hierarchical amyloid-like fibrils with multilayer structures, which effectively control the growth and lateral organization of hydroxyapatite within adaptive gaps. The resulting mineralized HSAF achieves a hardness of 0.616 ± 0.007 GPa and a modulus of 19.06 ± 3.54 GPa—properties closely resembling native hard tissues—and exhibits exceptionally high bioactivity in promoting both native bone tissue growth and further intrafibrillar mineralization, achieving 76.9% repair in a mice cranial defect model after 8 weeks and outperforming other regenerative materials. This remarkable performance, stemming from the unique structure and composition of the fibers, positions HSAF as a promising candidate for biomedical and engineering applications. These findings advance the understanding of biomineralization mechanisms and establish a foundation for developing high-bioactivity materials for hard tissue regeneration.
{"title":"Biomimetic Intrafibrillar Mineralization of Hierarchically Structured Amyloid-Like Fibrils","authors":"Shuting Miao, Jing Guo, Yuexin Zhang, Peisheng Liu, Xiaojie Chen, Qian Han, Yingbo Wang, Kun Xuan, Peng Yang, Fei Tao","doi":"10.1002/adma.202416824","DOIUrl":"https://doi.org/10.1002/adma.202416824","url":null,"abstract":"Intrafibrillar mineralization is essential not only as a fundamental process in forming biological hard tissues but also as a foundation for developing advanced composite fibril-based materials for innovative applications. Traditionally, only natural collagen fibrils have been shown to enable intrafibrillar mineralization, presenting a challenge in designing ordered hierarchical fibrils from common protein aggregation that exhibit similar high intrafibrillar mineralization activity. In this study, a mechanically directed two-step transformation method is developed that converts phase-transitioned protein nanofilms into crystalline, hierarchical amyloid-like fibrils with multilayer structures, which effectively control the growth and lateral organization of hydroxyapatite within adaptive gaps. The resulting mineralized HSAF achieves a hardness of 0.616 ± 0.007 GPa and a modulus of 19.06 ± 3.54 GPa—properties closely resembling native hard tissues—and exhibits exceptionally high bioactivity in promoting both native bone tissue growth and further intrafibrillar mineralization, achieving 76.9% repair in a mice cranial defect model after 8 weeks and outperforming other regenerative materials. This remarkable performance, stemming from the unique structure and composition of the fibers, positions HSAF as a promising candidate for biomedical and engineering applications. These findings advance the understanding of biomineralization mechanisms and establish a foundation for developing high-bioactivity materials for hard tissue regeneration.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"30 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798427","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}
引用次数: 0
Engineering Lattice Distortion in Ruthenium Oxide Enables Robust Acidic Water Oxidation via Direct O–O Coupling
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202500449
Yin'an Zhu, Fei Wu, Xiaozan Zhang, Yichao Lin, Linjuan Zhang, Ting-Shan Chan, Qiuju Zhang, Liang Chen
Ruthenium is considered one of the most promising alternatives to iridium as an anode electrocatalyst for proton exchange membrane water electrolysis (PEMWE). However, Ru-based electrocatalysts suffer from poor stability, primarily due to structural collapse under the harsh acidic conditions of oxygen evolution reaction (OER). Here, a design strategy is introduced that significantly enhances both the stability and activity of RuO2 by switching the catalytic mechanism from the adsorbate evolution mechanism (AEM) to the oxide pathway mechanism (OPM). This is achieved through lattice distortion engineering using a co-doping strategy involving large-radius ions (Na⁺ and Hf 4+). The incorporation of Na+ and Hf 4+ into RuO2 induces significant lattice distortion, shortening partial Ru─Ru bond distance and optimizing the electronic structure. This modification facilitates direct O–O radical coupling, as confirmed by in situ vibrational measurements and theoretical calculations. It can drive a current density of 1 A cm−2 in a PEMWE device at 60 °C with 1.646 V and operates stably for 85 h at 0.5 A cm−2. The present study highlights that optimizing the synergistic interaction between two adjacent Ru sites to promote direct O–O coupling is an effective strategy for enhancing the acidic OER performance of RuO2.
{"title":"Engineering Lattice Distortion in Ruthenium Oxide Enables Robust Acidic Water Oxidation via Direct O–O Coupling","authors":"Yin'an Zhu, Fei Wu, Xiaozan Zhang, Yichao Lin, Linjuan Zhang, Ting-Shan Chan, Qiuju Zhang, Liang Chen","doi":"10.1002/adma.202500449","DOIUrl":"https://doi.org/10.1002/adma.202500449","url":null,"abstract":"Ruthenium is considered one of the most promising alternatives to iridium as an anode electrocatalyst for proton exchange membrane water electrolysis (PEMWE). However, Ru-based electrocatalysts suffer from poor stability, primarily due to structural collapse under the harsh acidic conditions of oxygen evolution reaction (OER). Here, a design strategy is introduced that significantly enhances both the stability and activity of RuO<sub>2</sub> by switching the catalytic mechanism from the adsorbate evolution mechanism (AEM) to the oxide pathway mechanism (OPM). This is achieved through lattice distortion engineering using a co-doping strategy involving large-radius ions (Na⁺ and Hf <sup>4+</sup>). The incorporation of Na<sup>+</sup> and Hf <sup>4+</sup> into RuO<sub>2</sub> induces significant lattice distortion, shortening partial Ru─Ru bond distance and optimizing the electronic structure. This modification facilitates direct O–O radical coupling, as confirmed by in situ vibrational measurements and theoretical calculations. It can drive a current density of 1 A cm<sup>−2</sup> in a PEMWE device at 60 °C with 1.646 V and operates stably for 85 h at 0.5 A cm<sup>−2</sup>. The present study highlights that optimizing the synergistic interaction between two adjacent Ru sites to promote direct O–O coupling is an effective strategy for enhancing the acidic OER performance of RuO<sub>2</sub>.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"15 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789591","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}
引用次数: 0
Acceptor Crystallinity Engineering Enables >20% Efficiency Binary Organic Solar Cells with 83.0% Fill Factor
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202501243
Jiawei Deng, Wenhao Li, Rui Zeng, Jiali Song, Senke Tan, Lixuan Kan, Zhao Qin, Yan Zhao, Feng Liu, Yanming Sun
For spontaneously crystallized organic photovoltaic materials, morphology optimization remains a challenge due to the disparity in crystallinity between the donor and acceptor components. Imperfections in the crystalline phases result in significant trap-assisted recombination, which emerges as a critical factor limiting the fill factor (FF) of organic solar cells (OSCs). Herein, a method is introduced for precise regulation of the acceptor crystallinity, utilizing a novel upper-layer acceptor processing solvent, trichloroethylene (TCE), to improve the state and vertical morphology of the active layer. The TCE solvent synergistically optimizes intermolecular interactions among acceptor molecules and balances the film-forming process, thereby increasing the proportion of transport phases and forming high-speed channels for electron transport, which subsequently reduces trap-assisted charge recombination. As a result, the photovoltaic efficiency of binary organic solar cells reaches 20.05%. More importantly, an unprecedented FF of 83.0% is obtained, representing the highest FF value for OSCs. This facile and effective approach offers a promising means for constructing efficient charge transport networks and fabricating high-efficiency and morphologically stable OSCs.
对于自发结晶的有机光伏材料而言,由于供体和受体成分之间的结晶度差异,形态优化仍然是一项挑战。结晶相的不完美会导致严重的陷阱辅助重组,成为限制有机太阳能电池填充因子(FF)的关键因素。本文介绍了一种精确调节受体结晶度的方法,利用新型上层受体加工溶剂三氯乙烯(TCE)来改善活性层的状态和垂直形态。TCE 溶剂能协同优化受体分子间的相互作用,平衡成膜过程,从而增加传输相的比例,形成电子传输的高速通道,进而减少陷阱辅助电荷重组。因此,二元有机太阳能电池的光电效率达到了 20.05%。更重要的是,获得了史无前例的 83.0% 的 FF 值,代表了 OSCs 的最高 FF 值。这种简便有效的方法为构建高效的电荷传输网络和制造高效且形态稳定的 OSCs 提供了一种前景广阔的途径。
{"title":"Acceptor Crystallinity Engineering Enables >20% Efficiency Binary Organic Solar Cells with 83.0% Fill Factor","authors":"Jiawei Deng, Wenhao Li, Rui Zeng, Jiali Song, Senke Tan, Lixuan Kan, Zhao Qin, Yan Zhao, Feng Liu, Yanming Sun","doi":"10.1002/adma.202501243","DOIUrl":"https://doi.org/10.1002/adma.202501243","url":null,"abstract":"For spontaneously crystallized organic photovoltaic materials, morphology optimization remains a challenge due to the disparity in crystallinity between the donor and acceptor components. Imperfections in the crystalline phases result in significant trap-assisted recombination, which emerges as a critical factor limiting the fill factor (FF) of organic solar cells (OSCs). Herein, a method is introduced for precise regulation of the acceptor crystallinity, utilizing a novel upper-layer acceptor processing solvent, trichloroethylene (TCE), to improve the state and vertical morphology of the active layer. The TCE solvent synergistically optimizes intermolecular interactions among acceptor molecules and balances the film-forming process, thereby increasing the proportion of transport phases and forming high-speed channels for electron transport, which subsequently reduces trap-assisted charge recombination. As a result, the photovoltaic efficiency of binary organic solar cells reaches 20.05%. More importantly, an unprecedented FF of 83.0% is obtained, representing the highest FF value for OSCs. This facile and effective approach offers a promising means for constructing efficient charge transport networks and fabricating high-efficiency and morphologically stable OSCs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"73 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789628","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}
引用次数: 0
High Entropy Alloy Formation Derived from High Entropy Oxide: Unlocking the Active Sites for Green Methanol Production from CO2
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202504180
Devender Goud, Madhurima Sarkar, Harishankar Kopperi, Amitabha Das, Bitan Ray, Sreelakshmi Vijayaraghavan, Biswarup Pathak, Sebastian C Peter
In pursuit of novel materials for CO2 conversion to value-added chemicals, previous research has predominantly focused on copper-based, indium oxide (In2O3)-based, and alloy or intermetallic materials. However, a groundbreaking approach is presented by introducing a high-entropy-based material for CO2 reduction to methanol (CH3OH). This method offers scalability and simplicity, making it feasible for large-scale production of high-entropy-alloys (HEAs). The formation of HEA is facilitated by the presence of Fe, leads to the creation of a high-entropy oxide (HEO) during calcination. Through X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS), comprehensively analyzed the oxidation states and coordination environments of all metals in both HEO and HEA. The formation of Fe3O4 within the HEO structure is evident, with each metal occupying either tetrahedral (Td) or octahedral (Oh) sites. The HEA formed shows exceptional CO2 conversion efficiency and higher CH3OH selectivity. Isolated sites of Co, Ni with Fe, Cu, and Zn, along with CuZn pair, are considered as the active sites for CO2 to CH3OH and further determined by DFT calculations. The altered reaction mechanism upon HEA formation compared to individual metals is investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Finally, Life-cycle assessment (LCA) indicates the carbon-negative footprint.
{"title":"High Entropy Alloy Formation Derived from High Entropy Oxide: Unlocking the Active Sites for Green Methanol Production from CO2","authors":"Devender Goud, Madhurima Sarkar, Harishankar Kopperi, Amitabha Das, Bitan Ray, Sreelakshmi Vijayaraghavan, Biswarup Pathak, Sebastian C Peter","doi":"10.1002/adma.202504180","DOIUrl":"https://doi.org/10.1002/adma.202504180","url":null,"abstract":"In pursuit of novel materials for CO<sub>2</sub> conversion to value-added chemicals, previous research has predominantly focused on copper-based, indium oxide (In<sub>2</sub>O<sub>3</sub>)-based, and alloy or intermetallic materials. However, a groundbreaking approach is presented by introducing a high-entropy-based material for CO<sub>2</sub> reduction to methanol (CH<sub>3</sub>OH). This method offers scalability and simplicity, making it feasible for large-scale production of high-entropy-alloys (HEAs). The formation of HEA is facilitated by the presence of Fe, leads to the creation of a high-entropy oxide (HEO) during calcination. Through X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS), comprehensively analyzed the oxidation states and coordination environments of all metals in both HEO and HEA. The formation of Fe<sub>3</sub>O<sub>4</sub> within the HEO structure is evident, with each metal occupying either tetrahedral (T<sub>d</sub>) or octahedral (O<sub>h</sub>) sites. The HEA formed shows exceptional CO<sub>2</sub> conversion efficiency and higher CH<sub>3</sub>OH selectivity. Isolated sites of Co, Ni with Fe, Cu, and Zn, along with CuZn pair, are considered as the active sites for CO<sub>2</sub> to CH<sub>3</sub>OH and further determined by DFT calculations. The altered reaction mechanism upon HEA formation compared to individual metals is investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Finally, Life-cycle assessment (LCA) indicates the carbon-negative footprint.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"21 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798459","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}
引用次数: 0
TOP-Zn Steric Hindrance Effect Enables Ultra-Uniform CsPbX3 Quantum Dots for Wide-Color Gamut Displays
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202409308
Xinyi Lv, Yuqin Su, Hengyang Xiang, Linxiang Yang, Xinrui Chen, Yifei Wang, Kun Zhang, Jiahao Tang, Yuhui Ye, Bo Cai, Xueying Ma, Xiaoyong Wang, Haibo Zeng
Perovskite quantum dots (PQDs) are expected to be an ideal candidate for wide-color gamut displays owing to their high color purity. However, their color purity is challenged by remarkable spectral broadening due to non-uniform size distribution and crystal defects. Here, a ligand-ion (TOP-Zn) complex-modulating nucleation strategy is proposed to depress spectral broadening. This is achieved by enhancing the steric hindrance effect during lead-halogen octahedral assembly and reducing the reaction activity/sites of the system. This strategy is universal and has been confirmed to be effective for blue, green, and red PQDs, achieving narrowed spectral full-width-at-half-maximum (FWHM) of 15, 17, and 25 nm, respectively. These FWHMs are record-breaking and contribute to a wide color gamut coverage of ≈130% National Television Standards Committee and ≈100% Rec. 2020 standard. Meanwhile, these PQD-based light-emitting diodes (PeLEDs) exhibit a high external quantum efficiency (EQE) of exceeding 20% at their pure color range. These results provide a feasible path to achieve ultra-uniform and pure-color luminescent PQDs for wide-color gamut displays.
{"title":"TOP-Zn Steric Hindrance Effect Enables Ultra-Uniform CsPbX3 Quantum Dots for Wide-Color Gamut Displays","authors":"Xinyi Lv, Yuqin Su, Hengyang Xiang, Linxiang Yang, Xinrui Chen, Yifei Wang, Kun Zhang, Jiahao Tang, Yuhui Ye, Bo Cai, Xueying Ma, Xiaoyong Wang, Haibo Zeng","doi":"10.1002/adma.202409308","DOIUrl":"https://doi.org/10.1002/adma.202409308","url":null,"abstract":"Perovskite quantum dots (PQDs) are expected to be an ideal candidate for wide-color gamut displays owing to their high color purity. However, their color purity is challenged by remarkable spectral broadening due to non-uniform size distribution and crystal defects. Here, a ligand-ion (TOP-Zn) complex-modulating nucleation strategy is proposed to depress spectral broadening. This is achieved by enhancing the steric hindrance effect during lead-halogen octahedral assembly and reducing the reaction activity/sites of the system. This strategy is universal and has been confirmed to be effective for blue, green, and red PQDs, achieving narrowed spectral full-width-at-half-maximum (FWHM) of 15, 17, and 25 nm, respectively. These FWHMs are record-breaking and contribute to a wide color gamut coverage of ≈130% National Television Standards Committee and ≈100% Rec. 2020 standard. Meanwhile, these PQD-based light-emitting diodes (PeLEDs) exhibit a high external quantum efficiency (EQE) of exceeding 20% at their pure color range. These results provide a feasible path to achieve ultra-uniform and pure-color luminescent PQDs for wide-color gamut displays.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"31 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789592","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}
引用次数: 0
Chiroferromagnetic Quantum Dots for Chiroptical Synapse (ChiropS)
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202415366
Junyoung Kwon, Jae Bum Jeon, Walber Gonçalves Guimarães Júnior, Min Gu Lee, Changhyeon Lee, Geunyoung Kim, Hanchan Song, Woon Hyung Cheong, Sung Gap Im, André F. de Moura, Kyung Min Kim, Jihyeon Yeom
Optoelectronic devices using circularly polarized light (CPL) offer enhanced sensitivity and specificity for efficient data processing. There is a growing demand for CPL sensing mediums with strong optical activity, stability and sensitivity, multiple transition bands, and environmental compatibility. Here, defect-engineered chiroferromagnetic quantum dots (CFQDs) are used as a new type of CPL sensing material. By inducing amorphization defects through chiral molecules, CFQDs with high unpaired electron density, atomic structural chirality, amplified chiroptical activity, and multiple exciton transition bands are developed. CFQDs enable nonlinear, long-term plastic behavior with linear optical input, acting as in situ noise filters that reduce noise by over 20%. Additionally, CFQDs provide over nine times higher integration for photon polarization and wavelength distinctions, paving the way for next-generation processors with improved energy efficiency, integration, and reduced retention time.
{"title":"Chiroferromagnetic Quantum Dots for Chiroptical Synapse (ChiropS)","authors":"Junyoung Kwon, Jae Bum Jeon, Walber Gonçalves Guimarães Júnior, Min Gu Lee, Changhyeon Lee, Geunyoung Kim, Hanchan Song, Woon Hyung Cheong, Sung Gap Im, André F. de Moura, Kyung Min Kim, Jihyeon Yeom","doi":"10.1002/adma.202415366","DOIUrl":"https://doi.org/10.1002/adma.202415366","url":null,"abstract":"Optoelectronic devices using circularly polarized light (CPL) offer enhanced sensitivity and specificity for efficient data processing. There is a growing demand for CPL sensing mediums with strong optical activity, stability and sensitivity, multiple transition bands, and environmental compatibility. Here, defect-engineered chiroferromagnetic quantum dots (CFQDs) are used as a new type of CPL sensing material. By inducing amorphization defects through chiral molecules, CFQDs with high unpaired electron density, atomic structural chirality, amplified chiroptical activity, and multiple exciton transition bands are developed. CFQDs enable nonlinear, long-term plastic behavior with linear optical input, acting as in situ noise filters that reduce noise by over 20%. Additionally, CFQDs provide over nine times higher integration for photon polarization and wavelength distinctions, paving the way for next-generation processors with improved energy efficiency, integration, and reduced retention time.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"4 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789627","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}
引用次数: 0
Light-Driven Metal Exsolution-Redissolution of High-Entropy Oxide Enabling High-Performance Dry Reforming of Methane
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202500928
Cong Guo, Yu Cui, Wenqing Zhang, Xiaoyan Du, Xia Peng, Yue Yu, Jing Li, Yilin Wu, Yucheng Huang, Tingting Kong, Yujie Xiong
Solar-driven dry reforming of methane (DRM) is attractive for syngas production as an energy-efficient and environmentally friendly process. However, the remaining challenges of low yield and coke-induced inability in this route severely limit its applicability. Here, a light-induced metal exsolution-dissolution strategy is reported using high-entropy oxide (HEO) as a support for highly active and durable photothermal DRM. As evidenced by structural characterizations and theoretical simulations, the metal exsolution-dissolution process triggers the chemical looping of oxygen vacancies on HEO, in which CH4 is activated to CO and H2 by lattice oxygen while oxygen from CO2 can fill the oxygen vacancy and release CO. Such a pathway greatly improves product formation and coking resistance, overcoming the limitations. As a result, the optimized CoNiFeZnCr-HEO supported Rh nanocomposite achieves a high H2/CO production of 0.242/0.246 mol g−1 h−1 with a balance selectivity of 0.98 and impressive long-term stability (200 h). The yield is ≈300 and 450 times higher than that of quaternary and ternary oxides-based catalysts, respectively. This work paves the way for new insights into the light-driven DRM process and highlights the integration of dynamic surface evolution with molecular activation to enhance catalytic performance.
{"title":"Light-Driven Metal Exsolution-Redissolution of High-Entropy Oxide Enabling High-Performance Dry Reforming of Methane","authors":"Cong Guo, Yu Cui, Wenqing Zhang, Xiaoyan Du, Xia Peng, Yue Yu, Jing Li, Yilin Wu, Yucheng Huang, Tingting Kong, Yujie Xiong","doi":"10.1002/adma.202500928","DOIUrl":"https://doi.org/10.1002/adma.202500928","url":null,"abstract":"Solar-driven dry reforming of methane (DRM) is attractive for syngas production as an energy-efficient and environmentally friendly process. However, the remaining challenges of low yield and coke-induced inability in this route severely limit its applicability. Here, a light-induced metal exsolution-dissolution strategy is reported using high-entropy oxide (HEO) as a support for highly active and durable photothermal DRM. As evidenced by structural characterizations and theoretical simulations, the metal exsolution-dissolution process triggers the chemical looping of oxygen vacancies on HEO, in which CH<sub>4</sub> is activated to CO and H<sub>2</sub> by lattice oxygen while oxygen from CO<sub>2</sub> can fill the oxygen vacancy and release CO. Such a pathway greatly improves product formation and coking resistance, overcoming the limitations. As a result, the optimized CoNiFeZnCr-HEO supported Rh nanocomposite achieves a high H<sub>2</sub>/CO production of 0.242/0.246 mol g<sup>−1</sup> h<sup>−1</sup> with a balance selectivity of 0.98 and impressive long-term stability (200 h). The yield is ≈300 and 450 times higher than that of quaternary and ternary oxides-based catalysts, respectively. This work paves the way for new insights into the light-driven DRM process and highlights the integration of dynamic surface evolution with molecular activation to enhance catalytic performance.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"73 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789603","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}
引用次数: 0
All-Fiber 2 µm Mamyshev Oscillator: Mapping of Different Operating Regimes
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/lpor.202500074
Song Yang, Callum Robertson Smith, Christian Rosenberg Petersen, Ole Bang
The Mamyshev oscillator is an elegant and versatile method for generating ultrashort and high-energy laser pulses. It is realized in an all-fiber structure, which provides robustness and good beam quality, ensuring reliable and efficient performance. An all-fiber 2 µm Mamyshev oscillator is presented based on two Tm-doped fiber amplifiers separated by a broadband fixed wavelength filter with 11.2 nm −3 dB bandwidth and a tunable narrow bandwidth filter with 1.1 nm −3 dB bandwidth. Three distinct emission regimes are identified and mapped out in terms of the pump power and the filter wavelength separation: 1) no mode-locking if either pump power is insufficient 2) stable mode-locking in a limited region of pump powers, and 3) noise-like pulse mode-locking if one of the pump powers exceeds a threshold. It is demonstrated how the mode-locking region in terms of the two pump powers narrows with increasing filter wavelength separation and the pulses are compressed to 309 fs in standard silica fiber. The map over operation regimes provides a clear relationship between operating regimes and cavity parameters, offering valuable insights into the design of Mamyshev oscillators using filters of significantly different bandwidths.
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引用次数: 0
Friction Behavior and Microscopic Mechanism of Hydrogels in an Open-Air Environment
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202417177
Wenbo Zhu, Jiaqi Li, Feng Du, Nannan Jian, Jiuling Wang, Kai Zhang
Hydrogels composed of a solvent-saturated, cross-linked polymer network exhibit unique interfacial rheology and ultralow friction, making them valuable in biomedical applications. Despite their widespread use in open-air environments, the lubrication behaviors of hydrogels under these conditions remain poorly understood. Here, the microscopic mechanisms underlying the friction characteristics of hydrogels through a combination of experiments, theoretical analyses, and molecular dynamics simulations is explored. It is found that water evaporation from the hydrogel surface reduces the hydrodynamic layer thickness and increases surface viscosity, leading to a gradual rise in friction. On the other hand, optimizing pore size and water mobility within the hydrogel enhances water transport from the interior to the surface, mitigating evaporation and enabling consistently low friction. It is also explored how soaking time, water affinity, and applied normal load influence hydrogel lubrication. The findings elucidate the microscopic mechanisms governing the friction behaviors of hydrogels and provide guidelines for designing hydrogel systems with sustained exceptional lubrication properties in open-air applications.
由溶剂饱和的交联聚合物网络组成的水凝胶具有独特的界面流变性和超低摩擦性,因此在生物医学应用中具有重要价值。尽管水凝胶广泛应用于露天环境,但人们对其在这些条件下的润滑行为仍然知之甚少。本文通过实验、理论分析和分子动力学模拟相结合的方法,探讨了水凝胶摩擦特性的微观机制。研究发现,水凝胶表面的水分蒸发会减少水动力层厚度并增加表面粘度,从而导致摩擦力逐渐增大。另一方面,优化水凝胶内部的孔隙大小和水的流动性可增强水从内部向表面的传输,从而减少蒸发,并使摩擦力持续降低。研究还探讨了浸泡时间、水亲和力和施加的法向载荷如何影响水凝胶润滑。研究结果阐明了支配水凝胶摩擦行为的微观机制,并为设计在露天应用中具有持续优异润滑特性的水凝胶系统提供了指导。
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引用次数: 0
Improving the Stability of Wide Bandgap Perovskites: Mechanisms, Strategies, and Applications in Tandem Solar Cells
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-07 DOI: 10.1002/adma.202418500
Wenye Jiang, Yingjie Zhu, Jin Liu, Wenhan Yang, Hairui Cai, Bin Wang, Zhendong Sha, Guangkui Xu, Nan Zhang, Shengchun Yang, Chao Liang
Tandem solar cells (TSCs) based on wide bandgap (WBG) perovskites have gained significant attention for their higher power conversion efficiency (PCE) compared to single-junction cells. The role of WBG perovskite solar cells (PSCs) as the sub-cell in tandem cells consists of absorbing high-energy photons and producing higher open-circuit voltages (VOC). However, WBG PSCs face serious phase separation issues, resulting in poor long-term stability and substantial VOC loss in TSCs. In response, researchers have developed a range of strategies to mitigate these challenges, showing promising progress, and a comprehensive review of these strategies is expected. In this review, we discuss the stability mechanism in organic–inorganic hybrids and all-inorganic WBG perovskites. Additionally, we conduct an in-depth investigation of various strategies to enhance stability, including component engineering, additive engineering, interface engineering, dimension control, solvent engineering, and encapsulation. Furthermore, the application of the WBG sub-cell in various TSCs is summarized in detail. Finally, perspectives are provided to offer guidance for the development of efficient and stable WBG sub-cell in the field of TSCs.
{"title":"Improving the Stability of Wide Bandgap Perovskites: Mechanisms, Strategies, and Applications in Tandem Solar Cells","authors":"Wenye Jiang, Yingjie Zhu, Jin Liu, Wenhan Yang, Hairui Cai, Bin Wang, Zhendong Sha, Guangkui Xu, Nan Zhang, Shengchun Yang, Chao Liang","doi":"10.1002/adma.202418500","DOIUrl":"https://doi.org/10.1002/adma.202418500","url":null,"abstract":"Tandem solar cells (TSCs) based on wide bandgap (WBG) perovskites have gained significant attention for their higher power conversion efficiency (PCE) compared to single-junction cells. The role of WBG perovskite solar cells (PSCs) as the sub-cell in tandem cells consists of absorbing high-energy photons and producing higher open-circuit voltages (<i>V</i><sub>OC</sub>). However, WBG PSCs face serious phase separation issues, resulting in poor long-term stability and substantial <i>V</i><sub>OC</sub> loss in TSCs. In response, researchers have developed a range of strategies to mitigate these challenges, showing promising progress, and a comprehensive review of these strategies is expected. In this review, we discuss the stability mechanism in organic–inorganic hybrids and all-inorganic WBG perovskites. Additionally, we conduct an in-depth investigation of various strategies to enhance stability, including component engineering, additive engineering, interface engineering, dimension control, solvent engineering, and encapsulation. Furthermore, the application of the WBG sub-cell in various TSCs is summarized in detail. Finally, perspectives are provided to offer guidance for the development of efficient and stable WBG sub-cell in the field of TSCs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"35 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789593","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}
引用次数: 0
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Advanced Materials
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