Advanced Materials

Chen, Dechao; Gao, Tianyu; Wei, Zengxi; Wang, Mengjia; Ma, Yingfei; Xiao, Dongdong; Cao, Changsheng; Lee, Cheng‐You; Liu, Pan; Wang, Dengchao; Zhao, Shuangliang; Wang, Hsiao‐Tsu; Han, Lili

2024 Advanced Materials

doi: 10.1002/adma.202410537

Maximizing the catalytic activity of single‐atom and nanocluster catalysts through the modulation of the interaction between these components and the corresponding supports is crucial but challenging. Herein, guided by theoretical calculations, a nanoporous bilayer WS2 Moiré superlattices (MSLs) supported Au nanoclusters (NCs) adjacent to Ru single atoms (SAs) (Ru1/Aun‐2LWS2) is developed for alkaline hydrogen evolution reaction (HER) for the first time. Theoretical analysis suggests that the induced robust electronic metal–support interaction effect in Ru1/Aun‐2LWS2 is prone to promote the charge redistribution among Ru SAs, Au NCs, and WS2 MSLs support, which is beneficial to reduce the energy barrier for water adsorption and thus promoting the subsequent H2 formation. As feedback, the well‐designed Ru1/Aun‐2LWS2 electrocatalyst exhibits outstanding HER performance with high activity (η10 = 19 mV), low Tafel slope (35 mV dec−1), and excellent long‐term stability. Further, in situ, experimental studies reveal that the reconstruction of Ru SAs/NCs with S vacancies in Ru1/Aun‐2LWS2 structure acts as the main catalytically active center, while high‐valence Au NCs are responsible for activating and stabilizing Ru sites to prevent the dissolution and deactivation of active sites. This work offers guidelines for the rational design of high‐performance atomic‐scale electrocatalysts.

Chen, Ding; Mu, Shichun

2024 Advanced Materials

doi: 10.1002/adma.202408285pmid: 39246151

A breakthrough in manufacturing procedures often enables people to obtain the desired functional materials. For the field of energy conversion, designing and constructing catalysts with high cost‐effectiveness is urgently needed for commercial requirements. Herein, the molten salt‐assisted synthesis (MSAS) strategy is emphasized, which combines the advantages of traditional solid and liquid phase synthesis of catalysts. It not only provides sufficient kinetic accessibility, but effectively controls the size, morphology, and crystal plane features of the product, thus possessing promising application prospects. Specifically, the selection and role of the molten salt system, as well as the mechanism of molten salt assistance are analyzed in depth. Then, the creation of the catalyst by the MSAS and the electrochemical energy conversion related application are introduced in detail. Finally, the key problems and countermeasures faced in breakthroughs are discussed and look forward to the future. Undoubtedly, this systematical review and insights here will promote the comprehensive understanding of the MSAS and further stimulate the generation of new and high efficiency catalysts.

Hung, Nguyen Tuan; Okabe, Ryotaro; Chotrattanapituk, Abhijatmedhi; Li, Mingda

2024 Advanced Materials

doi: 10.1002/adma.202409175pmid: 39263754

Optical properties in solids, such as refractive index and absorption, hold vast applications ranging from solar panels to sensors, photodetectors, and transparent displays. However, first‐principles computation of optical properties from crystal structures is a complex task due to the high convergence criteria and computational cost. Recent progress in machine learning shows promise in predicting material properties, yet predicting optical properties from crystal structures remains challenging due to the lack of efficient atomic embeddings. Here, Graph Neural Network for Optical spectra prediction (GNNOpt) is introduced, an equivariant graph‐neural‐network architecture featuring universal embedding with automatic optimization. This enables high‐quality optical predictions with a dataset of only 944 materials. GNNOpt predicts all optical properties based on the Kramers‐Krönig relations, including absorption coefficient, complex dielectric function, complex refractive index, and reflectance. The trained model is applied to screen photovoltaic materials based on spectroscopic limited maximum efficiency and search for quantum materials based on quantum weight. First‐principles calculations validate the efficacy of the GNNOpt model, demonstrating excellent agreement in predicting the optical spectra of unseen materials. The discovery of new quantum materials with high predicted quantum weight, such as SiOs, which host exotic quasiparticles with multifold nontrivial topology, demonstrates the potential of GNNOpt in predicting optical properties across a broad range of materials and applications.

Li, Hongxia; Hu, Yanan; Zhang, Yan; Zhang, Hao; Yao, Dong; Lin, Yuehe; Yan, Xu

2024 Advanced Materials

doi: 10.1002/adma.202409090pmid: 39225445

Metal‐halide perovskites have become attractive nanomaterials for advanced biosensors, yet the structural design remains challenging due to the trade‐off between environmental stability and sensing sensitivity. Herein, a trinity strategy is proposed to address this issue by integrating Mn (II) substitution with CsPb2Cl5 inert shell and NH2‐PEG‐COOH coating for designing Mn2+‐doped CsPbCl3/CsPb2Cl5 core/shell hetero perovskite nanocrystals (PMCP PNCs). The trinity strategy isolates the emissive Mn2+‐doped CsPbCl3 core from water and the Mn2+ d–d transition generates photoluminescence with a long lifetime, endowing the NH2‐PEG‐COOH capped Mn2+‐doped CsPbCl3/CsPb2Cl5 PNCs with robust water stability and oxygen‐sensitive property. Given the structural integration, photoluminescent hydrogel biosensors are designed by embedding the PMCP PNCs into the hydrogel system to deliver on‐site pesticide information on food products. Impressively, benefiting from the dual enzyme triggered‐responsive property of PMCP PNCs, the hydrogel biosensor is endowed with ultra‐high sensitivity toward chlorpyrifos pesticide at the nanogram per milliliter level. Such a robust PMCP PNCs‐based hydrogel sensor can provide accurate pesticide information while guiding the construction of photoluminescent biosensors for upcoming on‐site applications.

Meng, Fanbo; Ren, Yujin; Ping, Bu; Huang, Jin; Li, Peng; Chen, Xihao; Wang, Ning; Li, Hui; Zhang, Lei; Zhang, Siwen; Hu, Yingfang; Yu, Zhi Gen; Yin, Bosi; Ma, Tianyi

2024 Advanced Materials

doi: 10.1002/adma.202408475pmid: 39235588

Compact batteries and electronic devices offer a plethora of advantages, including space optimization, portability, integration capability, responsiveness, and reliability. These attributes are crucial technical enablers for the design and implementation of various electronic devices and systems within scientific exploration. Thus, the group harnesses additive manufacturing technology, specifically utilizing five‐axis curved‐surface multi‐material printing equipment, to fabricate aqueous zinc‐ion batteries with tungsten‐doped manganese dioxide cathode for enhanced adaptability and customization. The five‐axis linkage motion system facilitates shorter ion transportation paths for compact batteries and ensures precise and efficient molding of non‐developable curved surfaces. Afterward, the compact cell is integrated with a printed nano‐silver serpentine resistor temperature sensor, and an integrated functional circuit is created using intense‐pulse sintering. Incorporating an emitting Light Emitting Diode (LED) allows temperature measurement through variations in LED brightness. The energy storage module with a high degree of conformity on the carrier surface has the advantages of small size and improved space utilization. The capability to produce Zinc‐ion batteries (ZIBs) on curved surfaces presents new avenues for innovation in energy storage technologies, paving the way for the realization of flexible and conformal power sources.

Jang, Woongsik; Luong, Hoang M.; Kim, Min Soo; Nguyen, Thuc‐Quyen; Wang, Dong Hwan

2024 Advanced Materials

doi: 10.1002/adma.202406316pmid: 39246216

Organic photodetectors (OPDs) have received considerable attention owing to their superior absorption coefficient and tunable bandgap. The introduction of bulk‐heterojunction (BHJ) structure aims to maximize charge generation, however, its response speed is constrained by the random distribution of donor and acceptor. Herein, a multiple‐active layer design consisting of a single acceptor layer and a bulk‐heterojunction layer (A/BHJ structure) is introduced, which combines the benefits of both the planar junction and the BHJ, improving photo‐sensing. A transfer process is employed for this structure, which involves calculating the energy release rate at each interface, considering temperature and velocity. Consequently, the OPD with the A/BHJ structure is successfully fabricated through transfer printing, resulting in reduced dark current, superior detectivity (1.06 × 1013 Jones), and rapid response, achieved by creating a high hole injection barrier and suppressing trap sites within the interfaces. By thoroughly investigating charge dynamics in the structure, the A/BHJ structure‐based OPD attains large bandwidth detection with high signal‐to‐noise. An efficient wireless data communication system with digital‐to‐analog conversion is showcased using the A/BHJ structure‐based OPD.

Lee, Michelle M. S.; Yu, Eric Y.; Chau, Joe H. C.; Lam, Jacky W. Y.; Kwok, Ryan T. K.; Tang, Ben Zhong

2024 Advanced Materials

doi: 10.1002/adma.202407707pmid: 39246197

Bacteria share a longstanding and complex relationship with humans, playing a role in protecting gut health and sustaining the ecosystem to cause infectious diseases and antibiotic resistance. Luminogenic materials that share aggregation‐induced emission (AIE) characteristics have emerged as a versatile toolbox for bacterial studies through fluorescence visualization. Numerous research efforts highlight the superiority of AIE materials in this field. Recent advances in AIE materials in bacterial studies are categorized into four areas: understanding bacterial interactions, antibacterial strategies, diverse applications, and synergistic applications with bacteria. Initial research focuses on visualizing the unseen bacteria and progresses into developing strategies involving electrostatic interactions, amphiphilic AIE luminogens (AIEgens), and various AIE materials to enhance bacterial affinity. Recent progress in antibacterial strategies includes using photodynamic and photothermal therapies, bacterial toxicity studies, and combined therapies. Diverse applications from environmental disinfection to disease treatment, utilizing AIE materials in antibacterial coatings, bacterial sensors, wound healing materials, etc., are also provided. Finally, synergistic applications combining AIE materials with bacteria to achieve enhanced outcomes are explored. This review summarizes the developmental trend of AIE materials in bacterial studies and is expected to provide future research directions in advancing bacterial methodologies.

Shi, Baimei; Qu, Aihua; Li, Zongda; Xiong, Yingcai; Ji, Jianjian; Xu, Liguang; Xu, Chuanlai; Sun, Maozhong; Kuang, Hua

2024 Advanced Materials

doi: 10.1002/adma.202408090pmid: 39221522

This study aimed to develop an intranasal nanovaccine by combining chiral nanoparticles with the RSV pre‐fusion protein (RSV protein) to create L‐nanovaccine (L‐Vac). The results showed that L‐NPs increased antigen attachment in the nasal cavity by 3.83 times and prolonged its retention time to 72 h. In vivo experimental data demonstrated that the intranasal immunization with L‐Vac induced a 4.86‐fold increase in secretory immunoglobulin A (sIgA) secretion in the upper respiratory tract, a 1.85‐fold increase in the lower respiratory tract, and a 20.61‐fold increase in RSV‐specific immunoglobin G (IgG) titer levels in serum, compared with the commercial Alum Vac, while the neutralizing activity against the RSV authentic virus is 1.66‐fold higher. The mechanistic investigation revealed that L‐Vac activated the tumor necrosis factor (TNF) signaling pathway in nasal epithelial cells (NECs), in turn increasing the expression levels of interleukin‐6 (IL‐6) and C–C motif chemokine ligand 20 (CCL20) by 1.67‐fold and 3.46‐fold, respectively, through the downstream nuclear factor kappa‐B (NF‐κB) signaling pathway. Meanwhile, CCL20 recruited dendritic cells (DCs) and L‐Vac activated the Toll‐like receptor signaling pathway in DCs, promoting IL‐6 expression and DCs maturation, and boosted sIgA production and T‐cell responses. The findings suggested that L‐ Vac may serve as a candidate for the development of intranasal medicine against various types of respiratory infections.

Li, Yan; Liu, Changjiang; Zheng, Hong; Jiang, Jidong Samuel; Zhu, Zihua; Yan, Xi; Cao, Hui; Narayanachari, K.V.L.V.; Paudel, Binod; Koirala, Krishna Prasad; Zhang, Zhan; Fisher, Brandon; Wang, Huanhua; Karapetrova, Evguenia; Sun, Chengjun; Kelly, Shelly; Phelan, Daniel; Du, Yingge; Buchholz, Bruce; Mitchell, J. F.; Bhattacharya, Anand; Fong, Dillon D.; Zhou, Hua

2024 Advanced Materials

doi: 10.1002/adma.202402484pmid: 39219216

Topotactic reduction is critical to a wealth of phase transitions of current interest, including synthesis of the superconducting nickelate Nd0.8Sr0.2NiO2, reduced from the initial Nd0.8Sr0.2NiO3/SrTiO3 heterostructure. Due to the highly sensitive and often damaging nature of the topotactic reduction, however, only a handful of research groups have been able to reproduce the superconductivity results. A series of in situ synchrotron‐based investigations reveal that this is due to the necessary formation of an initial, ultrathin layer at the Nd0.8Sr0.2NiO3 surface that helps to mediate the introduction of hydrogen into the film such that apical oxygens are first removed from the Nd0.8Sr0.2NiO3 / SrTiO3 (001) interface and delivered into the reducing environment. This allows the square‐planar / perovskite interface to stabilize and propagate from the bottom to the top of the film without the formation of interphase defects. Importantly, neither geometric rotations in the square planar structure nor significant incorporation of hydrogen within the films is detected, obviating its need for superconductivity. These findings unveil the structural basis underlying the transformation pathway and provide important guidance on achieving the superconducting phase in reduced nickelate systems.

2024 Advanced Materials

doi: 10.1002/adma.202412792pmid: 39267387