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991.
Qiaomu Wang Kaifei Tang Qiaobo Liao Yang Xu Haocheng Xu Yandong Wang Peng Wang Zhen Meng Kai Xi 《Advanced functional materials》2023,33(6):2211356
Covalent organic frameworks (COFs) with various topologies are typically synthesized by selecting and designing connecting units with rich shapes. However, this process is time-consuming and labour-intensive. Besides, the tight stacking of COFs layers greatly restrict their structural advantages. It is crucial to effectively exploit the high porosity and active sites of COFs by topological design. Herein, for the first time, inducing in situ topological changes in sub-chemometric COFs by adding graphene oxide (GO) without replacing the monomer, is proposed. Surprisingly, GO can slow down the intermolecular stacking and induce rearrangement of COFs nanosheets. The channels of D- [4+3] COFs are significantly altered while the stacking of periodically expanded framework is weakened. This not only maximizes the exposure of pore area and polar groups, but also shortens the channels and increases the redox activity, which enables high loading while enhancing host-guest interactions. This topological transformation to exhibit the structural features of COFs for efficient application is an innovative molecular design strategy. 相似文献
992.
Fenglei Lyu Bingyun Ma Xulan Xie Daqi Song Yuebin Lian Hao Yang Wei Hua Hao Sun Jun Zhong Zhao Deng Tao Cheng Yang Peng 《Advanced functional materials》2023,33(26):2214609
Cobalt phthalocyanine (CoPc) anchored on heterogeneous scaffold has drawn great attention as promising electrocatalyst for carbon dioxide reduction reaction (CO2RR), but the molecule/substrate interaction is still pending for clarification and optimization to maximize the reaction kinetics. Herein, a CO2RR catalyst is fabricated by affixing CoPc onto the Mg(OH)2 substrate primed with conductive carbon, demonstrating an ultra-low overpotential of 0.31 ± 0.03 V at 100 mA cm−2 and high faradaic efficiency of >95% at a wide current density range for CO production, as well as a heavy-duty operation at 100 mA cm−2 for more than 50 h in a membrane electrode assembly. Mechanistic investigations employing in situ Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy unravel that Mg(OH)2 plays a pivotal role to enhance the CO2RR kinetics by facilitating the first-step electron transfer to form anionic *CO2− intermediates. DFT calculations further elucidate that introducing Lewis acid sites help to polarize CO2 molecules absorbed at the metal centers of CoPc and consequently lower the activation barrier. This work signifies the tailoring of catalyst-support interface at molecular level for enhancing the turnover rate of CO2RR. 相似文献
993.
Kai Li Wenxiu Xu Yi Chen Xiaoyi Liu Lanbo Shen Junkun Feng WeiWei Zhao Wenjun Wang Junling Wu Baojin Ma Shaohua Ge Hong Liu Jianhua Li 《Advanced functional materials》2023,33(28):2214522
Treating bacterial biofilm infections on implanted materials remains challenging in clinical practice, as bacteria can be resistant by weakening the host defense from immune cells like macrophages. Herein, a metal-piezoelectric hetero-nanostructure with mechanical energy-driven antimicrobial property is in situ constructed on the Ti implant. Under ultrasonic irradiation, the formed piezotronic Ti (piezoTi) can promote the generation of reactive oxygen species (ROS) by facilitating local charge transfer at the surface, thus leading to piezodynamic killing of Staphylococcus aureus (S. aureus) while downregulating biofilm-forming genes. In addition, the stimulated macrophages on piezoTi display potent phagocytosis and anti-bacterial activity through the activation of PI3K-AKT and MAPK pathway. As a demonstration, one-time ultrasound irradiation of piezoTi pillar implanted in an osteomyelitis model efficiently eliminates the S. aureus biofilm infection and rescues the implant with enhanced osteointegration. By the synergistic effect of ultrasound-driven piezodynamic therapy and immuno-regulation, the proposed piezoelectric nanostructured surface can endow Ti implants with highly efficient antibacterial performance in an antibiotic-free, noninvasive, and on-demand manner. 相似文献
994.
Junwei Xiang Chuanzhou Han Jianhang Qi Yanjie Cheng Kai Chen Yongming Ma Jiayu Xie Yue Hu Anyi Mei Yinhua Zhou Hongwei Han 《Advanced functional materials》2023,33(25):2300473
Due to the low cost and excellent potential for mass production, printable mesoscopic perovskite solar cells (p-MPSCs) have drawn a lot of attention among other device structures. However, the low open-circuit voltage (VOC) of such devices restricts their power conversion efficiency (PCE). This limitation is brought by the high defect density at perovskite grain boundaries in the mesoporous scaffold, which results in severe nonradiative recombination and is detrimental to the VOC. To improve the perovskite crystallization process, passivate the perovskite defects, and enhance the PCE, additive engineering is an effective way. Herein, a polymeric Lewis base polysuccinimide (PSI) is added to the perovskite precursor solution as an additive. It improves the perovskite crystallinity and its carbonyl groups strongly coordinate with Pb2+, which can effectively passivate defects. Additionally, compared with its monomer, succinimide (SI), PSI serves as a better defect passivator because the long-chained macromolecule can be firmly anchored on those defect sites and form a stronger interaction with perovskite grains. As a result, the champion device has a PCE of 18.84%, and the VOC rises from 973 to 1030 mV. This study offers a new strategy for fabricating efficient p-MPSCs. 相似文献
995.
Chi Guo Kang Du Runming Tao Yaqing Guo Shuhao Yao Jianxing Wang Deyu Wang Jiyuan Liang Shih-Yuan Lu 《Advanced functional materials》2023,33(29):2301111
Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO2 not only accelerates Li+ transport but also regulates Li+ solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF-rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE-based Li||Cu half-cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm−2 and 3 mAh cm−2, respectively. In addition, Li||LiFePO4 full-cells with a LM anode of limited Li supply of 4 mAh cm−2 achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g−1). Especially, when further applied in anode-free LMBs, the carbon cloth||LiFePO4 full-cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C. 相似文献
996.
Jiafeng Zhu Qingyuan Bi Yinghao Tao Wenyao Guo Jinchen Fan Yulin Min Guisheng Li 《Advanced functional materials》2023,33(15):2213131
Designing and developing visible-light-responsive materials for solar to chemical energy is an efficient and promising approach to green and sustainable carbon-neutral energy systems. Herein, a facile in situ growth hydrothermal strategy using Mo-modified ZnIn2S4 (Mo-ZIS) nanosheets coupled with NiTiO3 (NTO) microrods to synthesize multifunctional Mo-modified ZIS wrapped NTO microrods (Mo-ZIS@NTO) photocatalyst with enhanced interfacial electric field (IEF) effect and typical S-scheme heterojunction is reported. Mo-ZIS@NTO catalyst possesses wide-spectrum light absorption properties, excellent visible light-to-thermal energy effect, electron mobility, charges transfer, and strong IEF and exhibits excellent solar-to-chemical energy conversion for efficient visible-light-driven photocatalytic hydrogen evolution. Notably, the engineered Mo1.4-ZIS@NTO catalyst exhibits superior performance with H2 evolution rate of up to 14.06 mmol g−1 h− 1 and the apparent quantum efficiency of 44.1% at 420 nm. The scientific explorations provide an in-depth understanding of microstructure, S-scheme heterojunction, enhanced IEF, Mo-dopant facilitation effect. Moreover, the theoretical simulations verify the critical role of Mo element in promoting the adsorption and activation of H2O molecules, modulating the H adsorption behavior on active S sites, and thus accelerating the overall catalytic efficiency. The photocatalytic hydrogen evolution mechanism via S-scheme heterojunction with adjustable IEF regulation over Mo1.4-ZIS@NTO is also demonstrated. 相似文献
997.
Jine Zhang Xiaobing Chen Mengqin Wang Qinghua Zhang Wenxiao Shi Xiaozhi Zhan Meng Zhao Zhe Li Jie Zheng Hui Zhang Furong Han Huaiwen Yang Tao Zhu Banggui Liu Fengxia Hu Baogen Shen Yuansha Chen Yue Zhang Yunzhong Chen Weisheng Zhao Jirong Sun 《Advanced functional materials》2023,33(41):2306434
Ferromagnetic materials with a strong spin-orbit coupling (SOC) have attracted much attention in recent years because of their exotic properties and potential applications in energy-efficient spintronics. However, such materials are scarce in nature. Here, a proximity-induced paramagnetic to ferromagnetic transition for the heavy transition metal oxide CaRuO3 in (001)-(LaMnO3/CaRuO3) superlattices is reported. Anomalous Hall effect is observed in the temperature range up to 180 K. Maximal anomalous Hall conductivity and anomalous Hall angle are as large as ∼15 Ω−1 cm−1 and ∼0.93%, respectively, by one to two orders of magnitude larger than those of the typical 3d ferromagnetic oxides such as La0.67Sr0.33MnO3. Density functional theory calculations indicate the existence of avoid band crossings in the electronic band structure of the ferromagnetic CRO layer, which enhances Berry curvature thus strong anomalous Hall effects. Further evidences from polarized neutron reflectometry show that the CaRuO3 layers are in a fully ferromagnetic state (∼0.8 μB/Ru), in sharp contrast to the proximity-induced canted antiferromagnetic state in 5d oxides SrIrO3 and CaIrO3 (∼0.1 μB/Ir). More than that, the magnetic anisotropy of the (001)-(LaMnO3/CaRuO3) superlattices is eightfold symmetric, showing potential applications in the technology of multistate data storage. 相似文献
998.
Xinbo Guo Ning Li Yushu Xu Jianfu Zhao Fucai Cui Yimu Chen Xiaoyan Du Qinghai Song Guodong Zhang Xiao Cheng Xutang Tao Zhaolai Chen 《Advanced functional materials》2023,33(22):2213995
Metal halide perovskite single crystals are promising for diverse optoelectronic applications due to their outstanding properties. In comparison to the bulk, the crystal surface suffers from high defect density and is moisture sensitive; however, surface modification strategies of perovskite single crystals are relatively deficient. Herein, solar cells based on methylammonium lead triiodide (MAPbI3) thin single crystals are selected as a prototype to improve single-crystal perovskite devices by surface modification. The surface trap passivation and protection against moisture of MAPbI3 thin single crystals are achieved by one bifunctional molecule 3-mercaptopropyl(dimethoxy)methylsilane (MDMS). The sulfur atom of MDMS can coordinate with bare Pb2+ of MAPbI3 single crystals to reduce surface defect density and nonradiative recombination. As a result, the modified devices show a remarkable efficiency of 22.2%, which is the highest value for single-crystal MAPbI3 solar cells. Moreover, MDMS modification mitigates surface ion migration, leading to enhanced reverse-bias stability. Finally, the cross-link of silane molecules forms a protective layer on the crystal surface, which results in enhanced moisture stability of both materials and devices. This work provides an effective way for surface modification of perovskite single crystals, which is important for improving the performance of single-crystal perovskite solar cells, photodetectors, X-ray detectors, etc. 相似文献
999.
Youyu Duan Yang Wang Weixuan Zhang Jiangwei Zhang Chaogang Ban Danmei Yu Kai Zhou Jinjing Tang Xu Zhang Xiaodong Han Liyong Gan Xiaoping Tao Xiaoyuan Zhou 《Advanced functional materials》2023,33(28):2301729
Photocatalytic conversion of CO2 into fuels using pure water as the proton source is of immense potential in simultaneously addressing the climate-change crisis and realizing a carbon-neutral economy. Single-atom photocatalysts with tunable local atomic configurations and unique electronic properties have exhibited outstanding catalytic performance in the past decade. However, given their single-site features they are usually only amenable to activations involving single molecules. For CO2 photoreduction entailing complex activation and dissociation process, designing multiple active sites on a photocatalyst for both CO2 reduction and H2O dissociation simultaneously is still a daunting challenge. Herein, it is precisely construct Cu single-atom centers and two-coordinated N vacancies as dual active sites on CN (Cu1/N2CV-CN). Experimental and theoretical results show that Cu single-atom centers promote CO2 chemisorption and activation via accumulating photogenerated electrons, and the N2CV sites enhance the dissociation of H2O, thereby facilitating the conversion from COO* to COOH*. Benefiting from the dual-functional sites, the Cu1/N2CV-CN exhibits a high selectivity (98.50%) and decent CO production rate of 11.12 µmol g−1 h−1. An ingenious atomic-level design provides a platform for precisely integrating the modified catalyst with the deterministic identification of the electronic property during CO2 photoreduction process. 相似文献
1000.
Ya Lin Fanqi Meng Tao Zeng Qinghua Zhang Zhongqiang Wang Yankun Cheng Xiaoning Zhao Lin Gu Haiyang Xu Yichun Liu 《Advanced functional materials》2023,33(35):2302787
Direct observation of oxygen dynamics in an oxide-based second-order memristor can provide the valid evidence to clarify the memristive mechanism, however, which is still limited for now. In this study, the migration and diffusion of oxygen ions in the region of Pt/WO3-x Schottky interface are observed in the WO3-x second-order memristor by using the technique of in situ transmission electron microscopy (TEM) and the electron energy loss spectroscopy. Interestingly, the coexistence of memristive and memcapacitive switching can be implemented in this memristor. Combined with the analysis of depth-profile X-ray photoelectron spectroscopy (XPS), an interface-barrier-modulation second-order memristive model is proposed based on the above results. Notably, temporally correlative oxygen dynamics in the memristor offers the platform to integrate signals from multiple inputs, enabling the realization of the dendritic functions of synchronous and asynchronous integration for the application of logic operations with fault-tolerance capability and associative learning. These findings provide the experimental evidence to in-depth understanding of oxygen dynamics and switching mechanism in second-order memristor, which can support the optimization of memristive performance and the achievement of biorealistic synaptic functions. 相似文献