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991.
Zepan Wang Peiyuan Wu Xubing Zou Sheng Wang Lei Du Ting Ouyang Zhao-Qing Liu 《Advanced functional materials》2023,33(16):2214275
By using the more electro-negative Mn3+ ion to partially replace Co3+ at the octahedral site of spinel ZnCo2O4, i.e., forming ternary Zn–Mn–Co spinel oxide, the electrocatalytic oxygen reduction/evolution activity is found to be significantly increased. Considering the physical characterization and theoretical calculations, it demonstrated that the bond competition played a key role in regulating the cobalt valence state and the electrocatalytic activity. The partial replacement of octahedral-site-occupied Co3+ by Mn3+ can effectively modulate the adjacent Co–O bond and induce the Jahn–Teller effect, thus changing the originally stable crystal structure and optimizing the binding strength between the active center and reaction intermediates. Certainly, the Mn-substituted ZnMn1.4Co0.6O4/NCNTs exhibit higher electrocatalytic oxygen reduction reaction (ORR) activity than that of ZnCo2O4/NCNTs and ZnMn2O4/NCNTs, supporting that the Co–O bond covalency determines the ORR activity of spinel ZnCo2O4. This study offers the competition between adjacent Co–O and Mn–O bonds via the BOh–O–BOh edge-sharing geometry. The ion substitution at octahedral sites by less electronegative cations can be a new and effective way to improve the electrocatalytic performance of cobalt-based spinel oxides. 相似文献
992.
Gaoxue Jiang Jiandong Liu Jian He Huaping Wang Shihan Qi Junda Huang Daxiong Wu Jianmin Ma 《Advanced functional materials》2023,33(12):2214422
High-voltage lithium metal batteries (LMBs) are capable to achieve the increasing energy density. However, their cycling life is seriously affected by unstable electrolyte/electrode interfaces and capacity instability at high voltage. Herein, a hydrofluoric acid (HF)-removable additive is proposed to optimize electrode electrolyte interphases for addressing the above issues. N, N-dimethyl-4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) aniline (DMPATMB) is used as the electrolyte additive to induce PF6− decomposition to form a dense and robust LiF-rich solid electrolyte interphase (SEI) for suppressing Li dendrite growth. Moreover, DMPATMB can help to form highly Li+ conductive Li3N and LiBO2, which can boost the Li+ transport across SEI and cathode electrolyte interphase (CEI). In addition, DMPATMB can scavenge traced HF in the electrolyte to protect both SEI and CEI from the corrosion. As expected, 4.5 V Li|| LiNi0.6Co0.2Mn0.2O2 batteries with such electrolyte deliver 145 mAh g−1 after 140 cycles at 200 mA g−1. This work provides a novel insight into high-voltage electrolyte additives for LMBs. 相似文献
993.
Huimin Yu Deyu Wang Huanyu Jin Pan Wu Xuan Wu Dewei Chu Yi Lu Xiaofei Yang Haolan Xu 《Advanced functional materials》2023,33(24):2214828
Improving interfacial solar evaporation performance is crucial for the practical application of this technology in solar-driven seawater desalination. Lowering evaporation enthalpy is one of the most promising and effective strategies to significantly improve solar evaporation rate. In this study, a new pathway to lower vaporization enthalpy by introducing heterogeneous interactions between hydrophilic hybrid materials and water molecules is developed. 2D MoN1.2 nanosheets are synthesized and integrated with rGO nanosheets to form stacked MoN1.2-rGO heterostructures with massive junction interfaces for interfacial solar evaporation. Molecular dynamics simulation confirms that atomic thick 2D MoN1.2 and rGO in the MoN1.2-rGO heterostructures simultaneously interact with water molecules, while the interactions are remarkably different. These heterogeneous interactions cause an imbalanced water state, which easily breaks the hydrogen bonds between water molecules, leading to dramatically lowered vaporization enthalpy and improved solar evaporation rate (2.6 kg m−2 h−1). This study provides a promising strategy for designing 2D-2D heterostructures to regulate evaporation enthalpy to improve solar evaporate rate for clean water production. 相似文献
994.
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
995.
The complementary electrochromic device, where the optical transmittance changes upon the flow of cations back and forth between anodic and cathodic electrodes, operates in a rocking-chair fashion if it can inherently self-discharge. Herein, the first demonstration of a dual-mode electrochromic platform having self-coloring and self-bleaching characteristics is reported, which is realized by sandwiching zinc metal within a newly-designed Prussian blue (PB)-WO3 rocking-chair type electrochromic device. It is demonstrated that the redox potential differences between the zinc metal and the WO3/PB electrodes endow the self-color-switching of these electrodes. By employing a hybrid electrolyte of Zn2+/K+, it is further shown that the colored PB-WO3 rocking-chair device is capable of spontaneously bleaching when the anodic and cathodic electrodes are coupled. This dual-mode light-control strategy enables the electrochromic devices to exhibit four distinct optical states with the highest optical contrast of 72.6% and fast switching times (<5 s for the bleaching/coloration processes). Furthermore, the built-in voltage of the dual-mode electrochromic devices not only promotes energy efficiency, but also augments the bistability of the devices. It is envisioned that the broad implication of the present platform is in the development of self-powered smart windows, colorful displays, optoelectronic switches, and optical sensors. 相似文献
996.
Bolun Li Xi Huang Xiang Wu Qiong Zuo Yunhao Cao Qi Zhu Yaohui Li Yuanhuan Xu Guanhaojie Zheng Dongcheng Chen Xu-Hui Zhu Fei Huang Hongyu Zhen Lintao Hou Jian Qing Wanzhu Cai 《Advanced functional materials》2023,33(28):2300216
Quasi-two-dimensional (Q-2D) perovskites are emerging as one of the most promising materials for photodetectors. However, a significant challenge to Q-2D perovskites for photodetection is their insufficient charge transport ability, which is mainly attributed to their hybrid low-dimensional n-phase structure. This study demonstrates that evenly-distributed 3D-like phases with vertical orientation throughout the film can greatly facilitate charge transport and suppress charge recombination, outperforming the prevalent phase structure with a vertical dimension gradient. Based on such a phase structure, a Q-2D Ruddlesden−Popper perovskite self-powered photodetector achieving a combination of exceptional figures-of-merit is realized, including a responsivity of 0.45 AW−1, a peak specific detectivity of 2.3 × 1013 Jones, a 156 dB linear dynamic range, and a rise/fall time of 2.89 µs/1.93 µs. The desired phase structure is obtained by utilizing a double-hole transport layer (HTL), combining hydrophobic PTAA and hydrophilic PEDOT: PSS. Besides, the dependence of the hybrid low-dimensional phase structure is also identified on the surface energy of the buried HTL substrate. This study gives insight into the correlation between Q-2D perovskites’ phase structure and performance, providing a valuable design guide for Q-2D perovskite-based photodetectors. 相似文献
997.
Juan Li Jinhua Huang Yongjian Jiang Limin Wu Yonghui Deng 《Advanced functional materials》2023,33(8):2212317
Diverse diseases and increasing prevalence pose a serious threat to public health. Point-of-care testing (POCT) techniques have imposed superior requirements over sensitivity, selectivity, robustness, affordability, and high-throughput. However, transient signal, complex sample pretreatment, and low signal-to-noise ratio make POCT severely limited in detection accuracy, efficiency, and sensitivity. Here, an enzyme-assisted magnetic large-mesoporous nanoreactor (FS) is constructed for achieving persistent-chemiluminescence signal output and eliminating matrix interference in disease diagnosis. The core-shell structured FS synthesized via an interface coassembly method exhibits uniform size, large and open mesopores (≈22 nm), and intrinsic magnetic separability. Such unique FS acts as efficient nanoreactor for confined cascade reactions enable efficient persistent-chemiluminescence (pCL) signal transduction and high-SNR chromogenic analysis of diverse biomarkers. The developed pCL assays facilitate high-sensitive determination of chronic disease biomarkers glucose and uric acid with detection limits (DL) of 5.4 mg L−1 and 151.2 ng L−1, respectively. The proposed chromogenic immunoassay enables an ultrasensitive and visual determination of alpha-fetoprotein with a DL of 1.2 ng L−1, which is superior to previously published immunoassays. The feasibility of the developed methods for real-world applications are demonstrated in 159 clinical serum samples, and the determination results agree well with the clinical data. The proposed technique is expected to promote highly sensitive disease diagnosis in primary medical institutions and resource-limited areas since not relying on expensive automatic sampling and testing instruments. The good flexibility of the customizable nanoreactor makes it a powerful tool for developing various POCT techniques for rapid, sensitive, and accurate diseases diagnosis. 相似文献
998.
Kexin Wang Junhui Cao Xiaoxuan Yang Xiahan Sang Siyu Yao Rong Xiang Bin Yang Zhongjian Li Thomas O'Carroll Qinghua Zhang Lecheng Lei Gang Wu Yang Hou 《Advanced functional materials》2023,33(16):2212321
Designing hydrogen evolution reaction (HER) electrocatalysts for facilitating its sluggish adsorption kinetics is crucial in generating green hydrogen via sustainable water electrolysis. Herein, a high-performance ultra-low Ruthenium (Ru) catalyst is developed consisting of atomically-layered Ru nanoclusters with adjacent single Ru sites, which executs a bridging-Ru-H activation strategy to kinetically accelerate the HER elementary steps. Owing to its optimal electronic structure and unique adsorption configuration, the hybrid Ru catalyst simultaneously displayed a drastically reduced overpotential of 16 mV at 10 mA cm−2 as well as a low Tafel slope of 35.2 mV dec−1 in alkaline electrolyte. When further coupled with a commercial IrO2 anode catalyst, the ensembled anion-exchange membrane water electrolyzer achievs a current density of 1.0 A cm−2 at a voltage of only 1.70 Vcell. In situ spectroscopic analysis verified that Ru single atom and atomically-layered Ru nanoclusters in the hybrid materials play a critical role in facilitating water dissociation and weakening *H adsorption, respectively. Theoretical calculations further elucidate the underlaying mechanism, suggesting that the dissociated proton at the single atom Ru site orients itself adjacently with Ru nanoclusters in a bridged structure through targeted charge transfer, thus promoting Volmer-Heyrovsky dynamics and boosting the HER activity. 相似文献
999.
Zhongsheng Wang Chunlei Zhu Jiandong Liu Xinhong Hu Yulu Yang Shihan Qi Huaping Wang Daxiong Wu Junda Huang Pengbin He Jianmin Ma 《Advanced functional materials》2023,33(19):2212150
Tailoring inorganic components of cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) is critical to improving the cycling performance of lithium metal batteries. However, it is challenging due to complicated electrolyte reactions on cathode/anode surfaces. Herein, the species and inorganic component content of the CEI/SEI is enriched with an objectively gradient distribution through employing pentafluorophenyl 4-nitrobenzenesulfonate (PFBNBS) as electrolyte additive guided by engineering bond order with functional groups. In addition, a catalytic effect of LiNi0.6Mn0.2Co0.2O2 (NCM622) cathode is proposed on the decomposition of PFBNBS. PFBNBS with lower highest occupied molecular orbital can be preferentially oxidized on the NCM622 surface with the help of the catalytic effect to induce an inorganic-rich CEI for superior electrochemical performance at high voltage. Moreover, PFBNBS can be reduced on the Li surface due to its lower lowest unoccupied molecular orbital , increasing inorganic moieties in SEI for inhibiting Li dendrite generation. Thus, 4.5 V Li||NCM622 batteries with such electrolyte can retain 70.4% of initial capacity after 500 cycles at 0.2 C, which is attributed to the protective effect of the excellent CEI on NCM622 and the inhibitory effect of its derived CEI/SEI on continuous electrolyte decomposition. 相似文献
1000.
Haiping Wu Shun Huang Ying Zhu Jia Li Xiaoxiao Pang Yongyao Tang Siqiao Li Ping Ji Shijia Ding Wei Cheng Wenyang Li 《Advanced functional materials》2023,33(19):2212669
The accumulation of reactive oxygen species (ROS) and minimal osteogenic raw material in the osteoporotic bone microenvironment greatly inhibits the activity of osteoblasts. Herein, it is originally proposed to construct a biomatrix multifaceted bone microenvironment amendment -Mineralized zippered G4-Hemin DNAzyme hydrogel (MDH)-to improve osteoporotic osteogenic capacity and promote high-quality bone defect repair. The programmed design of the rolling circle amplified DNA hydrogel synthesis system allows the introduction of massive amounts of zippered G4-Hemin DNAzyme in MDH. The zippered G4-Hemin DNAzyme highly mimics the tight catalytic configuration of horseradish peroxidase and exerts excellent enzyme-like activity with considerable ROS molecule scavenging ability. In addition, the DNA amplification by-product pyrophosphate is ingeniously employed as a sufficient phosphorus source, thus constituting an autonomous mineralization system for waste reuse through the introduction of pyrophosphate hydrolase and calcium ions, which deposits in MDH as an osteogenic raw material and addresses the challenge of DNA hydrogel bio-application stability. The remarkable in vitro and in vivo outcomes demonstrate that MDH can effectively improve the oxidative stress status of osteoblasts, restore the balance of mitochondrial membrane potential, and reduce apoptosis, ultimately demonstrating superior osteogenic capacity. 相似文献