Tamanna Khan, Terry McAfee, Thomas J. Ferron, Awwad Alotaibi, Brian A. Collins
{"title":"Local Chemical Enhancement and Gating of Organic Coordinated Ionic-Electronic Transport","authors":"Tamanna Khan, Terry McAfee, Thomas J. Ferron, Awwad Alotaibi, Brian A. Collins","doi":"10.1002/adma.202406281","DOIUrl":"https://doi.org/10.1002/adma.202406281","url":null,"abstract":"Superior properties in organic mixed ionic-electronic conductors (OMIECs) over inorganic counterparts have inspired intense interest in biosensing, soft-robotics, neuromorphic computing, and smart medicine. However, slow ion transport relative to charge transport in these materials is a limiting factor. Here, it is demonstrated that hydrophilic molecules local to an interfacial OMIEC nanochannel can accelerate ion transport with ion mobilities surpassing electrophoretic transport by more than an order of magnitude. Furthermore, ion access to this interfacial channel can be gated through local surface energy. This mechanism is applied in a novel sensing device, which electronically detects and characterizes chemical reaction dynamics local to the buried channel. The ability to enhance ion transport at the nanoscale in OMIECs as well as govern ion transport through local chemical signaling enables new functionalities for printable, stretchable, and biocompatible mixed conduction devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"42 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672850","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}
Boqu Chen, Xiaoyu Sun, Xiaoxuan Li, Lu Cai, Ding Zhao, Kaikai Du, Meiyan Pan, Min Qiu
{"title":"4H-SiC Metalens: Mitigating Thermal Drift Effect in High-Power Laser Irradiation.","authors":"Boqu Chen, Xiaoyu Sun, Xiaoxuan Li, Lu Cai, Ding Zhao, Kaikai Du, Meiyan Pan, Min Qiu","doi":"10.1002/adma.202412414","DOIUrl":"10.1002/adma.202412414","url":null,"abstract":"<p><p>Enhancing energy density and efficiency in laser processing hinges on precise beam focusing, yet this often causes severe heat absorption and focus shifts in optical lenses. Traditional cooling methods increase cost and complexity, severely limiting versatility. Here, monolithic silicon carbide (SiC) metalens is introduced, which shows unparalleled thermal stability, integrated with a high-power laser. This metalens achieves diffraction-limited focusing with a numerical aperture (NA) of 0.5 and a focal length of 1 cm. Under a 1030 nm pulsed laser at 15 W for 1 h, it shows a minimal temperature rise of 3.2 °C and a tiny focal shift of 14 µm (0.1% relative), only 6% of the shift in conventional lenses. When used to cut a 4H-SiC substrate with the same laser, the metalens exhibit only an 11.4% change in cutting depth after 1 h of operation, correlating with the focal shift results. The results unveil a groundbreaking class of compact SiC photonics devices nearly impervious to heat absorption, representing a monumental leap for high-power laser systems and opening new horizons for their applications and efficiency.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2412414"},"PeriodicalIF":27.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666768","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}
Meng Dan, Shan Yu, Weihua Lin, Mohamed Abdellah, Zhen Guo, Zhao-Qing Liu, Tõnu Pullerits, Kaibo Zheng, Ying Zhou
{"title":"Balancing the Charge Separation and Surface Reaction Dynamics in Twin-Interface Photocatalysts for Solar-to-Hydrogen Production.","authors":"Meng Dan, Shan Yu, Weihua Lin, Mohamed Abdellah, Zhen Guo, Zhao-Qing Liu, Tõnu Pullerits, Kaibo Zheng, Ying Zhou","doi":"10.1002/adma.202415138","DOIUrl":"10.1002/adma.202415138","url":null,"abstract":"<p><p>Solar-driven photocatalytic green hydrogen (H<sub>2</sub>) evolution reaction presents a promising route toward solar-to-chemical fuel conversion. However, its efficiency has been hindered by the desynchronization of fast photogenerated charge carriers and slow surface reaction kinetics. This work introduces a paradigm shift in photocatalyst design by focusing on the synchronization of charge transport and surface reactions through the use of twin structures as a unique platform. With CdS twin structure (CdS-T) as a model, the role of twin boundaries in modulating surface reactions and facilitating charge migration is systematically investigated. Utilizing transient absorption (TA) and time-resolved infrared (TRIR) spectroscopies, it is revealed that CdS-T achieves charge separation on a picosecond timescale and, importantly, the surface reaction at the twin boundary with the involvement of holes also occurs within 100 ps to 3 ns. This synchronization of charge donation and surface regeneration significantly enhances the hydrogen evolution process. Accordingly, CdS-T exhibits superior activity for visible light photocatalytic H<sub>2</sub> production, withthe H<sub>2</sub> production rate of 55.61 mmol h<sup>-1</sup> g<sup>-1</sup> and remarkable stability (>30 h), outperforming pristine CdS significantly. This study underscores the transformative potential of twin structures in photocatalysis, offering a new avenue to synchronize charge transport and surface reactions.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2415138"},"PeriodicalIF":27.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666771","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}
Lixin Su, Hao Wu, Shaokun Zhang, Chenxi Cui, Shengnan Zhou, Huan Pang
{"title":"Insight Into Intermediate Behaviors and Design Strategies of Platinum Group Metal-Based Alkaline Hydrogen Oxidation Catalysts.","authors":"Lixin Su, Hao Wu, Shaokun Zhang, Chenxi Cui, Shengnan Zhou, Huan Pang","doi":"10.1002/adma.202414628","DOIUrl":"10.1002/adma.202414628","url":null,"abstract":"<p><p>Hydrogen oxidation reaction (HOR) can effectively convert the hydrogen energy through the hydrogen fuel cells, which plays an increasingly important role in the renewable hydrogen cycle. Nevertheless, when the electrolyte pH changes from acid to base, even with platinum group metal (PGM) catalysts, the HOR kinetics declines with several orders of magnitude. More critically, the pivotal role of reaction intermediates and interfacial environment during intermediate behaviors on alkaline HOR remains controversial. Therefore, exploring the exceptional PGM-based alkaline HOR electrocatalysts and identifying the reaction mechanism are indispensable for promoting the commercial development of hydrogen fuel cells. Consequently, the fundamental understanding of the HOR mechanism is first introduced, with emphases on the adsorption/desorption process of distinct reactive intermediates and the interfacial structure during catalytic process. Subsequently, with the guidance of reaction mechanism, the latest advances in the rational design of advanced PGM-based (Pt, Pd, Ir, Ru, Rh-based) alkaline HOR catalysts are discussed, focusing on the correlation between the intermediate behaviors and the electrocatalytic performance. Finally, given that the challenges standing in the development of the alkaline HOR, the prospect for the rational catalysts design and thorough mechanism investigation towards alkaline HOR are emphatically proposed.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2414628"},"PeriodicalIF":27.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666866","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}
Wenjie Yang, Chenglin Zheng, Li Sun, Zhiying Bie, Yuchen Yue, Xiuhong Li, Wentao Sun, Tomiki Ikeda, Jingxia Wang, Lei Jiang
{"title":"Spatiotemporal Programmability of 3D Chiral Color Units Driven by Ink Spontaneous Diffusion toward Customized Printing","authors":"Wenjie Yang, Chenglin Zheng, Li Sun, Zhiying Bie, Yuchen Yue, Xiuhong Li, Wentao Sun, Tomiki Ikeda, Jingxia Wang, Lei Jiang","doi":"10.1002/adma.202411988","DOIUrl":"https://doi.org/10.1002/adma.202411988","url":null,"abstract":"Blue phase liquid crystals (BPLCs) have exhibited promising applications in 3D flexible displays due to their molecular-level self-assembled chiral structures, fast response, and tunable polarized colors. However, there remain challenges for spatiotemporal programming of 3D chiral color units for BPLC dynamic patterning. Herein, the programmable temporal evolution of micrometer-scale color units and spatial configuration switch of chiral modes are achieved by spontaneous ink diffusion-driven asymmetric lattice deformation in dual-chiral polymer-templated blue phases. Custom-printed colorful patterns are designed by machine learning-assisted parameter optimization, which displays programmable multidimensional encrypted information that incorporates temporal evolving colors (wavelength), spatial distribution (depth), chiral modes (L/R). The quantitative relationship between ink diffusion kinetics and blue-phase dynamic 3D structural optics is established by in situ characterization, finite element analysis, and mathematical geometry modeling. This work provides insights into the microgeometric manipulation of 3D chiral color of BPLCs in the application of information security and self-adaptive indicators.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"18 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672857","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}
{"title":"Dual Near-Infrared-Response S-Scheme Heterojunction with Asymmetric Adsorption Sites for Enhanced Nitrogen Photoreduction.","authors":"Jiaxin Li, Chaoqi Zhang, Tong Bao, Yamin Xi, Ling Yuan, Yingying Zou, Yin Bi, Chao Liu, Chengzhong Yu","doi":"10.1002/adma.202416210","DOIUrl":"10.1002/adma.202416210","url":null,"abstract":"<p><p>Photocatalytic nitrogen reduction reaction (PNRR) holds immense promise for sustainable ammonia (NH<sub>3</sub>) synthesis. However, few photocatalysts can utilize NIR light that carries over 50% of the solar energy for NH<sub>3</sub> production with high performance. Herein, a dual NIR-responsive S-scheme ZnCoS<sub>x</sub>/Fe<sub>3</sub>S<sub>4</sub> heterojunction photocatalyst is designed with asymmetric adsorption sites and excellent PNRR performance. The heterojunction possesses a hollow-on-hollow superstructure: Fe<sub>3</sub>S<sub>4</sub> nanocrystal-modified ZnCoS<sub>x</sub> nanocages as building blocks assemble into spindle-shaped particles with a spindle-like cavity. Both Fe<sub>3</sub>S<sub>4</sub> and ZnCoS<sub>x</sub> are NIR active, allowing efficient utilization of full-spectrum light. Moreover, an S-scheme heterojunction is constructed that promotes charge separation. In addition, the Fe/Co dual-metal sites at the interface enable an asymmetric side-on adsorption mode of N<sub>2</sub>, favoring the polarization and activation of N<sub>2</sub> molecules. In combination with the promoted mass transfer and active site exposure of hollow superstructure, a superior PNRR performance is achieved, with a high NH<sub>3</sub> evolution rate of 2523.4 µmol g<sup>-1</sup> h<sup>-1</sup>, an apparent quantum yield of 9.4% at 400 nm and 8% at 1000 nm, and a solar-to-chemical conversion efficiency of 0.32%. The work paves the way for the rational design of advanced heterojunction catalysts for PNRR.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2416210"},"PeriodicalIF":27.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666773","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}
{"title":"Universal Approach for Managing Iodine Migration in Inverted Single-Junction and Tandem Perovskite Solar Cells.","authors":"Zhenhua Song, Kexuan Sun, Yuanyuan Meng, Zewei Zhu, Yaohua Wang, Weifu Zhang, Yang Bai, Xiaoyi Lu, Ruijia Tian, Chang Liu, Ziyi Ge","doi":"10.1002/adma.202410779","DOIUrl":"https://doi.org/10.1002/adma.202410779","url":null,"abstract":"<p><p>Despite significant progress in the power-conversion efficiency (PCE) of perovskite solar cells (PSCs), the instability of devices remains a considerable obstacle for commercial applications. This instability primarily originates from the migration of halide ions-particularly iodide ions (I<sup>-</sup>). Under light exposure and thermal stress, I<sup>-</sup> migrates and transforms into I<sub>2</sub>, leading to irreversible degradation and performance loss. To address this issue, we introduced the additive 2,1,3-benzothiadiazole,5,6-difluoro-4,7-bis(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) (BT2F-2B) into the perovskite. The strong coordination between the unhybridized p orbital and lone-pair electrons from I<sup>-</sup> inhibits the deprotonation of MAI/FAI and the subsequent conversion of I<sup>-</sup> to I₂. The highly electronegative fluorine enhances its electrostatic interaction with I<sup>-</sup>. Consequently, the synergistic effect of BT2F-2B effectively suppresses the decomposition of perovskite and the defect density of the iodide vacancies. This approach delivers a PCE over 26% for inverted single-junction PSCs, with exceptional operational stability. According to the ISOS-L-3 testing protocol (maximum power point tracking at 85 °C and 50% relative humidity), treated PSCs retain 85% of their original PCE after 1000 h of aging. When the BT2F-2B is applied to a wide-bandgap (1.77 eV) perovskite system, the PCE of all-perovskite tandem solar cells reaches 27.8%, confirming the universality of the proposed strategy.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2410779"},"PeriodicalIF":27.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646272","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}
{"title":"Field-Programmable Topographic-Morphing Array for General-Purpose Lab-on-a-Chip Systems.","authors":"Yangyang Fan, Huimin Wu, Jiao Wang, Jiu-An Lv","doi":"10.1002/adma.202410604","DOIUrl":"https://doi.org/10.1002/adma.202410604","url":null,"abstract":"<p><p>Lab-on-a-chip systems seek to leverage microfluidic chips to enable small-scale fluid manipulation, holding significant potential to revolutionize science and industry. However, existing microfluidic chips have been largely designed with static fluid structures for specific single-purpose applications, which lack adaptability and flexibility for diverse applications. Inspired by the general-purpose design strategy of the customizable chip of integrated circuit - field programmable gate array whose hardware can be reconfigured via software programming for multifunctionality after manufacturing, a conceptual-new reconfigurable microfluidic chip - field programmable topographic morphing array (FPTMA) is devised with exceptional structural reconfiguration, field programmability, and function scalability for general-purpose lab-on-a-chip systems that beyond the reach of current state-of-art lab-on-chip systems. FPTMA can be software programmed to dynamically shape an elastic meta-interface from the initial smooth structure into desired time-varying topographic structures and thus generate spatiotemporal topographic-morphing-induced capillary forces to actively manipulate multidroplets in parallel and enable real-time reconfiguring diverse microfluidic operations/functions/flow networks as well as workflows. It is envisioned that the development of the FPTMA-driven lab-on-a-chip systems that leverage dynamic interfacial topographies to digitally handle microfluidics would significantly stimulate numerous technological innovations in biology/medicine/chemistry.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2410604"},"PeriodicalIF":27.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646226","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}
Ipsita Nath, Jeet Chakraborty, Kuber Singh Rawat, Yanwei Ji, Rundong Wang, Korneel Molkens, Nathalie De Geyter, Rino Morent, Veronique Van Speybroeck, Pieter Geiregat, Pascal Van Der Voort
{"title":"Mesoporous Acridinium-Based Covalent Organic Framework for Long-lived Charge-Separated Exciton Mediated Photocatalytic [4+2] Annulation.","authors":"Ipsita Nath, Jeet Chakraborty, Kuber Singh Rawat, Yanwei Ji, Rundong Wang, Korneel Molkens, Nathalie De Geyter, Rino Morent, Veronique Van Speybroeck, Pieter Geiregat, Pascal Van Der Voort","doi":"10.1002/adma.202413060","DOIUrl":"https://doi.org/10.1002/adma.202413060","url":null,"abstract":"<p><p>Readily tuneable porosity and redox properties of covalent organic frameworks (COFs) result in highly customizable photocatalysts featuring extended electronic delocalization. However, fast charge recombination in COFs severely limits their photocatalytic activities. Herein a new mode of COF photocatalyst design strategy to introduce systematic trap states is programmed, which aids the formation and stabilization of long-lived charge-separated excitons. Installing cationic acridinium functionality in a pristine electron-rich triphenylamine COF via postsynthetic modification resulted in a semiconducting photocatalytic donor-acceptor dyad network that performed rapid and efficient oxidative Diels-Alder type [4+2] annulation of styrenes and alkynes to fused aromatic compounds under the atmospheric condition in good to excellent yields. Large mesopores of ≈4 nm diameter ensured efficient mass flow within the COF channel. It is confirmed that the catalytic performance of COF originates from the ultra-stable charge-separated excitons of 1.9 nm diameter with no apparent radiative charge-recombination pathway, endorsing almost a million times better photo-response and catalysis than the state-of-the-art.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2413060"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646238","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}
{"title":"Synergistic Modulation of Orientation and Steric Hindrance Induced by Alkyl Chain Length in Ammonium Salt Passivator Toward High-performance Inverted Perovskite Solar Cells and Modules.","authors":"Wenhuan Gao, Jike Ding, Quanxing Ma, Hong Zhang, Jiajia Zhang, Zuolin Zhang, Mengjia Li, Yang Wang, Boxue Zhang, Thierry Pauporté, Jian-Xin Tang, Jiangzhao Chen, Cong Chen","doi":"10.1002/adma.202413304","DOIUrl":"https://doi.org/10.1002/adma.202413304","url":null,"abstract":"<p><p>Organic ammonium salts are extensively utilized for passivating surface defects in perovskite films to mitigate trap-assisted nonradiative recombination. However, the influence of alkyl chain length on the molecular orientation and spatial steric hindrance of ammonium salt remains underexplored, hindering advancements in more effective passivators. Here, a series of organic ammonium salts is reported with varying alkyl chain lengths to passivate surface defects and optimize band alignment. It is revealed that long alkyl chains promote parallel molecular orientation on the perovskite surface, thereby reinforcing interaction with surface defects, whereas excessive chain length introduces steric hindrance, weakening anion-perovskite interactions. Nonylammonium acetate (NAAc) with optimal chain length achieves the ideal balance between chemical interactions, resulting in superior passivation. Through NAAc passivation, high-performance inverted perovskite solar cells (PSCs) and modules are achieved, with power conversion efficiencies (PCE) of 25.79% (certified 25.12%) and 19.62%, respectively. This marks a record PCE for inverted PSCs utilizing vacuum flash technology in ambient conditions. Additionally, the NAAc-passivated devices retain 91% of their initial PCE after 1200 h of continuous maximum power point operation. This work offers new insights into the interplay between molecular orientation and steric hindrance, advancing the design of high-performance PSCs.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2413304"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646210","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}