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Yuguang Chao Peng Zhou Jianping Lai Weiyu Zhang Huawei Yang Shiyu Lu Hui Chen Kun Yin Menggang Li Lu Tao Changshuai Shang Meiping Tong Shaojun Guo 《Advanced functional materials》2021,31(24):2100923
Designing a semiconductor-based heterostructure photocatalyst for achieving the efficient separation of photogenerated electron-hole pairs is highly important for enhancing H2 releasing photocatalysis. Here, a new class of Ni1−xCoxSe2–C/ZnIn2S4 hierarchical nanocages with abundant and compact ZnIn2S4 nanosheets/Ni1−xCoxSe2 C nanosheets 2D/2D hetero–interfaces, is designed and synthesized. The constructed heterostructure photocatalyst exposes rich hetero-junctions, supplying the broad and short transfer paths for charge carriers. The close contacts of these two kinds of nanosheets induce a strong interaction between ZnIn2S4 and Ni1−xCoxSe2 C, improving the separation and transfer of photo-generated electron-hole pairs. As a consequence, the distinctive Ni1−xCoxSe2 C/ZnIn2S4 hierarchical nanocages without using additional noble-metal cocatalysts, display remarkable H2-relaesing photocatalytic activity with a rate of 5.10 mmol g−1 h−1 under visible light irradiation, which is 6.2 and 30 times higher than those of fresh ZnIn2S4 nanosheets and bare Ni1−xCoxSe2 C nanocages, respectively. Spectroscopic characterizations and theory calculations reveal that the strong interaction between ZnIn2S4 and Ni1−xCoxSe2 C 2D/2D hetero-interfaces can powerfully promote the separation of photo-generated charge carriers and the electrons transfer from ZnIn2S4 to Ni1−xCoxSe2 C. 相似文献
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Kezhen Lai Yuxin Sun Ning Li Yangqin Gao Hui Li Lei Ge Tianyi Ma 《Advanced functional materials》2024,34(49):2409031
Photocatalytic conversion of CO2 to methane faces challenges due to the stability of CO2, unpredictable intermediates, and complex electron transfer steps. Herein, a spatial In2S3/In2O3 heterojunction with abundant S vacancies (ISIO(VS)) is obtained through facile Polyvinylpyrrolidone (PVP) treatment to reach a methane yield of 16.52 µmol·g−1·h−1 with a selectivity of 95.93%, which is the highest among reported In2S3 and In2O3 based catalysts. The work function (Wf), differential charge density, and Kelvin Probe Force Microscopy (KPFM) results confirm that S vacancies strengthen the built-in electric field (BEF) of In2S3/In2O3 (ISIO) heterojunctions, improving carrier separation. Density functional theory (DFT) calculations reveal that S vacancies induce electron redistribution, facilitating adsorption and activation of CO2 and *CO intermediate, thus promoting hydrogenation to yield *CHO. The reaction pathway of photocatalytic CO2 reduction is revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and Gibbs free energy (ΔG). The S vacancies modify electronic orbitals and the highest occupied molecular orbital (HOMO) of In atom, resulting in a stronger interaction between the catalyst and *CHO, which reduces ΔG*CHO and regulates the selectivity of CH4. This study paves a new avenue for the design of photocatalysts with highly selective reduction of CO2 to CH4 through defect engineering. 相似文献
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Kailian Zhang Meng Dan Jingfei Yang Fengxiu Wu Leigang Wang Hua Tang Zhao-Qing Liu 《Advanced functional materials》2023,33(35):2302964
Constructing rich defect active site structure for material design is still a great challenge. Herein, a simple surface engineering strategy is demonstrated to construct one-unit-cell ZnIn2S4 atomic layers with the modulated surface energy of S vacancy. Rich surface energy can regulate and control the rich S vacancy, which ensures rich active sites, higher charge density and effective carrier transport. As a result, the ZnIn2S4 atomic layers with rich surface energy affords an obvious enhancement in H2O2 productive rate of 1592.04 µmol g−1 h−1, roughly 14.58 times superior to that with poor surface energy. Moreover, the in situ infrared diffuse reflection spectrum indicates that S vacancy as the oxygen reduction reaction active site is responsible for the critical intermediate *O2− and *OOH, corresponding to two-electron oxygen reduction reaction. This study provides a valuable insight and guidance for constructing controllably defects to achieve highly efficient H2O2 production. 相似文献
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以硝酸铟为原料,尿素为沉淀剂,将反应物溶于乙二醇,放入聚四氟乙烯内衬的反应釜中于200℃反应,采用溶剂热法一步制得In2O3纳米粉体。研究了反应时间和温度对粉体的结构、表面形貌和粒度的影响,并初步探讨了反应机理。结果表明:所制粉体为类球形,平均粒径约为25 nm。制备过程无需高温煅烧、操作简单,所得产物纯度高、粒度均匀、分散性好。 相似文献
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Yiqiang He Heng Rao Kepeng Song Jixin Li Ying Yu Yue Lou Chunguang Li Yu Han Zhan Shi Shouhua Feng 《Advanced functional materials》2019,29(45)
Zinc vacancy (VZn) is successfully introduced into 3D hierarchical ZnIn2S4 (3D‐ZIS). The photo‐electrochemical experiments demonstrate that the charge separation and carrier transfer are more efficient in the 3D‐ZIS with rich VZn. Of note, for the first time, it is found that VZn can decrease the carrier transport activation energy (CTAE), from 1.14 eV for Bulk‐ZIS (Bulk ZnIn2S4) to 0.93 eV for 3D‐ZIS, which may provide a feasible platform for further understanding the mechanism of photocatalytic CO2 reduction. In situ Fourier transform infrared (FT‐IR) results reveal that the presence of rich VZn ensures CO2 chemical activation, promoting single‐electron reduction of CO2 to CO2?. In addition, in situ FT‐IR and CO2 temperature programmed desorption results show that VZn can promote the formation of surface hydroxyl. To the best of current knowledge, there are no reports on the photoreduction of CO2 simply by virtue of 3D‐ZIS with VZn and few literature reports on the photocatalytic reduction of CO2 concerned with CTAE. Additionally, this work finds that surface hydroxyl may play a crucial role in the process of CO2 photoreduction. The work may provide some novel ways to ameliorate solar energy conversion performance and a better understanding of photoreaction mechanisms. 相似文献
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采用反应蒸发技术制作不掺杂In2O3透明导电薄膜,薄膜厚度为150~200nm、方块电阻为60~200Ω/□,透光率为80%~94%(波长λ=600mm)。了蒸发过程氧气充入量和蒸发时间对薄膜的光电特性的影响,说明低蒸发速率和限制氧气流量是获得优质薄膜的关键。 相似文献
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Minghua Xu Xiaowen Ruan Depeng Meng Guozhen Fang Dongxu Jiao Shengli Zhao Zheyang Liu Zhifeng Jiang Kaikai Ba Tengfeng Xie Wei Zhang Jing Leng Shengye Jin Sai Kishore Ravi Xiaoqiang Cui 《Advanced functional materials》2024,34(37):2402330
The sustainable production of hydrogen utilizing solar energy is a pivotal strategy for reducing reliance on fossil fuels. ZnIn2S4 (ZIS), as a typical metal sulfide semiconductor, has received extensive attention in photocatalysis. Although the introduction of sulfur (S) vacancies in ZIS to enhance photocatalytic hydrogen production by creating defect energy levels has been explored, detailed studies on the control and modulation of S-vacancies in ZIS are sparce. This study demonstrates that while moderate levels of S-vacancies can enhance hydrogen evolution, excessive vacancies may hinder the process, underscoring the importance of S-vacancy modulation. Guided by theoretical calculations, We have designed and synthesized ZIS with modulated S-vacancies to realize favorable hydrogen adsorption-free energy and integrated in a Schottky-heterojunction with MXene co-catalysts for enhanced hydrogen evolution. The optimized hydrogen evolution performance of ZnIn2S4/MXene (ZMX) reaches 14.82 mmol g−1 h−1 under visible light irradiation, surpassing many reported ZnIn2S4-based photocatalysts. The enhanced performance is ascribed to widened light absorption and enhanced carrier transportation realized by S-vacancy modulation and the co-catalytic effect. Femtosecond ultrafast absorption (fs-TA) spectra and other in-situ/ex-situ characterizations further prove an efficient separation and transfer in an as-prepared ZMX catalyst. These findings open up new perspectives for designing catalysts with vacancy modulation. 相似文献
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采用水热法制备了质量分数w[La(NO3)3]为3%~9%的La(NO3)3-In2O3纳米粉体。利用XRD,SEM,TEM等测试手段,对其物相、结构进行了表征。结果表明:掺质量分数为7%的La(NO3)3的In2O3纳米粉体,其颗粒长度和直径分别为2μm与200nm左右,呈棒状。利用该纳米粉体制成气敏元件,并采用静态配气法测试了元件的气敏性能。研究发现:元件在110℃的工作温度下,对体积分数为100×10-6的Cl2的灵敏度高达1665.7,且具有良好的选择性与响应-恢复特性。 相似文献
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Ruixin Bian Yan Jiang Yuan Wang Jian‐Kun Sun Jinsong Hu Lei Jiang Huan Liu 《Advanced functional materials》2018,28(19)
Microbial extracellular electron transfer (EET) with high performance and good controllability is always desired in various bioelectric applications. Depending on the redox state, C‐type cytochromes located across the outer membranes (OMCs) mediate EET with different behaviors. Here, by incorporating Sn‐doped In2O3 nanowire array with flat F‐doped In2O3 (FTO), a composite electrode is developed that can highly boost EET by over 60 times at a certain potential of 0.2 V, where normally only limited EET current is observed on a conductive electrode. It is proposed that the underlay FTO with bias 0.2 V promotes EET via OMCs by physical contacting with microbes, while the semiconductor nanowires provide a suitable energy level to facilitate the EET via OMC‐flavins cofactor, breaking the stereotype of the certain redox state of OMCs at a given potential. As a synergistic effect, EET via both OMCs and flavins is highly boosted simultaneously to achieve the dual‐pathway EET, which could be further amplified by the nanostructured topology of the as‐prepared electrode. Moreover, the EET current shows a positive correlation with the nanowire length, showing good controllability. This work provides an applicable method for constructing various highly efficient bioelectric devices. 相似文献
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Yanwei Zhu Wenfang Deng Yueming Tan Jianqiao Shi Jingcheng Wu Wenbo Lu Jianfeng Jia Shuangyin Wang Yuqin Zou 《Advanced functional materials》2023,33(45):2304985
Photocatalytic selective oxidation of 5-hydroxymethylfurfural (HMF) coupled H2 production offers a promising approach to producing valuable chemicals. Herein, an efficient in situ topological transformation tactic is developed for producing porous O-doped ZnIn2S4 nanosheets for HMF oxidation cooperative with H2 evolution. Aberration-corrected high-angle annular dark-field scanning TEM images show that the hierarchical porous O-ZIS-120 possesses abundant atomic scale edge steps and lattice defects, which is beneficial for electron accumulation and molecule adsorption. The optimal catalyst (O-ZIS-120) exhibits remarkable performance with 2,5-diformylfuran (DFF) yields of 1624 µmol h−1 g−1 and the selectivity of >97%, simultaneously with the H2 evolution rate of 1522 µmol h−1 g−1. Mechanistic investigations through theoretical calculations show that O in the O-ZIS-120 lattice can reduce the oxidation energy barrier of hydroxyl groups of HMF. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) results reveal that DFF* (C4H2(CHO)2O*) intermediate has a weak interaction with O-ZIS-120 and desorb as the final product. This study elucidates the topotactic structural transitions of 2D materials simultaneously with electronic structure modulation for efficient photocatalytic DFF production. 相似文献
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Xuan Li Shuo Li Jiamin Tian Fengjiao Lyu Jianhui Liao Qing Chen 《Advanced functional materials》2024,34(3):2306486
2D layered semiconductors with excellent light−matter interaction and atomic-scale thickness have been envisioned as promising candidates for more than Moore and beyond Moore technologies. Here, for the first time, a multi-functional platform is reported that is fabricated entirely from wrinkle-free 2D ferroelectric semiconductor α-In2Se3 integrated with a photodetector, reconfigurable logic switching, and visual perception processing functions. The intensity- and wavelength-dependent resistance is used to demodulate broadband optical information into electrical signals and perform reconfigurable logic switching. Moreover, the platform offers dynamically modulated photosensitive visual sensing in different working modes at the pixel level. Using photo-assisted piezoresponse force microscopy, the optical-engineered ferroelectric polarization switch behavior is explored. The platform has excellent sensitivity to both optical and electrical stimuli and can respond to lights in the visible to short-wavelength infrared region in volatile/non-volatile manner under gate voltage modulation, with a response of 98 mA W−1 (to 1800 nm light), a current on/off ratio of over 106, and a high field-effect mobility of 137.55 cm2 V−1 s−1. With its simple structure, unique photoelectric interaction, and controllable operating mechanism, the platform has the potential to simplify the complexity of neuromorphic computing circuitry systems, paving the way for high-performance hybrid technologies suitable for artificial intelligence applications. 相似文献
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Hui Cheng Qiong Liu Yuwei Diao Liling Wei Jianghan Chen Fuxian Wang 《Advanced functional materials》2021,31(37):2103732
CoMo2S4 2D nanosheets are constructed by a hard template-limited domain strategy, meanwhile the hydrogen evolution reaction (HER) properties and the function of Co in CoMo2S4 are systematically investigated. Electrochemical tests show that CoMo2S4 possesses high HER performance with an overpotential of 55 and 150 mV at 10 and 100 mA cm−2, respectively, outperforming Pt/C (20%) and the state of art Mo–S, Co–S, and Co–Mo–S-based materials. An in-depth mechanism study reveals that the main active site of CoMo2S4 is Mo rather than Co, whereas Co plays a key role in improving the electrical conductivity of the catalyst and thus improving the HER performance. X-ray photoelectron spectroscopy and density of state tests demonstrate that the introduction of Co leads to electron delocalization in the catalyst, making the electrons transport easier and finally endowing the catalyst with better conductive performance. It is believed this is the first time that the effect of Co on improving the bulk conductivity of Co–Mo–S catalyst is proposed, which highlights the potency of Co in improving the electrocatalytic HER activity of Mo–S-based materials. 相似文献
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Yulin Zheng Xin Tang Wenliang Wang Ling Jin Guoqiang Li 《Advanced functional materials》2021,31(6):2008307
Following the extensive researches of graphene, 2D layered semiconductors have attracted widespread attention for their intriguing physical properties. 2D α-Ga2S3 as an important member of group IIIA–VIA semiconductors has outstanding optoelectronic properties. However, the controllable large-size synthesis of ultrathin α-Ga2S3 nanosheets still remains a huge challenge. In this paper, a large-size ultrathin nanosheets of hexagonal Ga2S3 is prepared via an improved chemical vapor deposition method. High-performance photodetectors based on the ultrathin Ga2S3 nanosheets is demonstrated. The device shows a high photosensitivity/detectivity (9.2 A W−1/1.4 × 1012 Jones) and a fast response time (rise/fall time of <4/3 ms), respectively. Strikingly, wearable flexible photodetectors based on Ga2S3 nanosheets are fabricated accordingly and demonstrate great response performance and stability. This work provides a new direction for 2D semiconductors to apply in next-generation nanoscale smart optoelectronics. 相似文献
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YU Zhou YANG Zhi-mei CHEN Hao WU Zhan-wen JIN Yong JIAO Zhi-feng HE Yi WANG Hui LIU Jun-gang GONG Min SUN Xiao-song 《半导体光子学与技术》2007,13(2):155-160
Ga2O3 nano-structures, nanowires and nanosheets are produced on Au pre coated(111) silicon substrates with chemical vapor deposition(CVD) technique. By evaporating pure Ga powder in the H2O atmosphere under ambient pressure the large-scale preparation of β-Ga2O3 with monoclinic crystalline structure is achieved. The crystalline structures and morphologies of produced Ga2O3 nano-structures are characterized by means of scanning electron microscope(SEM), X-ray diffraction(XRD), selected area electron diffraction (SAED) and transmission electron microscope(TEM). Raman spectrum reveals the typical vibration modes of Ga2O3 The vibration mode shifts corresponding to Ga2O3 nano-structures are not found. Two distinguish photoluminescence(PL) emissions are found at about 399 nm and 469 nm owing to the VO-VGa excitation and VO-VGaO excitation, respectively. The growth mechanisms of Ga2O3 nanowires and nanosheets are discussed with vapor liquid-solid(VLS) and vapor-solid(VS) mechanisms. 相似文献
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采用后硒化Cu-Zn-Sn-S电沉积预制层的方法制备了铜锌锡硫硒薄膜,其中Cu-Zn-Sn-S预制层是通过含有不同浓度的硫代硫酸钠电解液电沉积而成的.实验发现,硒化前后薄膜的性质与硫代硫酸钠浓度密切相关.SEM,EDS,XRD,Raman和透射光谱分析表明,当硫代硫酸钠的浓度为5 mM时,沉积的薄膜形貌平整,晶粒明显,组分贫锌,具有单一的铜锌锡硫硒结构,且其带隙为1.11 eV; 在浓度高于5 mM下沉积的薄膜形貌粗糙并产生杂相硒化锡; 在浓度低于5 mM下沉积的薄膜组分严重贫锌并生成大量的Cu2SnSe3. 相似文献