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< Page ,Total 11 >
Regulating the Scaling Relations in Ammonia Synthesis through a Light-Driven Bendable Seesaw Effect on Tailored Iron Catalyst SCIE
期刊论文 | 2024 , 63 (44) | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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Abstract :

Advancing the energy-intensive Haber-Bosch process faces significant challenges due to the intrinsic constraints of scaling relations in heterogeneous catalysis. Herein, we reported an approach of bending the "seesaw effect" to regulate the scaling relations over a tailored alpha-Fe metallic material (alpha-Fe-110s), realizing highly efficient light-driven thermal catalytic ammonia synthesis with a rate of 1260 mu mol gcatalyst-1 h-1 without additional heating. Specifically, the thermal catalytic activity of alpha-Fe-110s was significantly enhanced by the novel stepped {110} surface, exhibiting a 3.8-fold increase compared to the commercial fused-iron catalyst with promoters at 350 degrees C. The photo-induced hot electron transfer further accelerates the dinitrogen dissociation and hydrogenation simultaneously, effectively overcoming the limitation of scaling relation over identical sites. Consequently, the ammonia production rate of alpha-Fe-110s was further enhanced by 30 times at the same temperature with irradiation. This work designs an efficient and sustainable system for ammonia synthesis and provides a novel approach for regulating the scaling relations in heterogeneous catalysis. The stepped {110} surface of the prepared alpha-Fe-110s exposes abundant C7 sites with moderate EN, achieving a delicate balance in scaling relations and thermal catalytic activity for ammonia synthesis. A novel light-induced "bendable seesaw effect" resulting from hot electron transfer between catalyst and adsorbates was discovered to regulate the scaling relations and further significantly enhances the catalytic activity. image

Keyword :

photothermal catalysis photothermal catalysis alpha-Fe catalyst alpha-Fe catalyst ammonia synthesis ammonia synthesis hot electron transfer hot electron transfer scaling relations scaling relations

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GB/T 7714 Yang, Yi , Wang, Pei , Zhang, Xiaohu et al. Regulating the Scaling Relations in Ammonia Synthesis through a Light-Driven Bendable Seesaw Effect on Tailored Iron Catalyst [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (44) .
MLA Yang, Yi et al. "Regulating the Scaling Relations in Ammonia Synthesis through a Light-Driven Bendable Seesaw Effect on Tailored Iron Catalyst" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 44 (2024) .
APA Yang, Yi , Wang, Pei , Zhang, Xiaohu , Wang, Shengyao , Ding, Xing , Ma, Hongshan et al. Regulating the Scaling Relations in Ammonia Synthesis through a Light-Driven Bendable Seesaw Effect on Tailored Iron Catalyst . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (44) .
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Surficial Reconstruction of Pt-Ni/NiS and Its Effect on Electrocatalytic Hydrogen Evolution in Alkaline Medium SCIE
期刊论文 | 2024 , 16 (34) , 44879-44888 | ACS APPLIED MATERIALS & INTERFACES
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Abstract :

Cyclic voltammetry pretreatment of Pt-based electrocatalysts has been proven to be a normal activation process on achieving the optimal alkaline hydrogen evolution performance. Until now, the congruent relationship between the microstructural evolution and performance improvement during this process has rarely been reported. Herein, when the in situ transmission electron microscopy and in situ Raman analyses are employed, a self-reconstruction process from crystalline NiS into amorphous nickel hydroxide hydrate [Ni(OH)(2-x)H2O, where x approximate to 0.3] on the surface of platinum-nickel nanowires has first been captured, which is the critical water dissociation active site to offer a sufficient proton supply. Furthermore, such a surficial reconstruction triggers an increase in the current density from -2.3 to -38.8 mA/cm(2) (at -70 mV), which is nearly 17 times. These observations point to the fact that it is essential to consider the fundamental mechanisms of hydrogen evolution on the active sites when the process is scaled up.

Keyword :

in situ Raman in situ Raman hydrogen evolution reaction hydrogen evolution reaction in situ TEM in situ TEM surficial reconstruction surficial reconstruction Pt-based catalysis Pt-based catalysis

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GB/T 7714 Wang, Yueshuai , Zhao, Yuguo , Lu, Yue et al. Surficial Reconstruction of Pt-Ni/NiS and Its Effect on Electrocatalytic Hydrogen Evolution in Alkaline Medium [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (34) : 44879-44888 .
MLA Wang, Yueshuai et al. "Surficial Reconstruction of Pt-Ni/NiS and Its Effect on Electrocatalytic Hydrogen Evolution in Alkaline Medium" . | ACS APPLIED MATERIALS & INTERFACES 16 . 34 (2024) : 44879-44888 .
APA Wang, Yueshuai , Zhao, Yuguo , Lu, Yue , Huang, Guoyu , Shen, Zhitong , Selvakumar, Karuppaiah et al. Surficial Reconstruction of Pt-Ni/NiS and Its Effect on Electrocatalytic Hydrogen Evolution in Alkaline Medium . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (34) , 44879-44888 .
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Strongly-Confined CsPbI3 Quantum Dots by Surface Cleaning-Induced Ligand Exchange for Spectrally Stable Pure-Red Light-Emitting Diodes with Efficiency Exceeding 26% SCIE
期刊论文 | 2024 , 6 (9) , 4115-4123 | ACS MATERIALS LETTERS
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Abstract :

The advancement of pure-red perovskite light-emitting diodes (PeLEDs) is still a challenge because of surface "wastes" (like surface vacancies and excessive insulating ligands) on quantum dots (QDs). Herein, we develop a method to synthesize single-halide pure-red CsPbI3 QDs, combining a strong quantum confinement effect and meticulous surface-cleaning-induced ligand exchange. We achieve pure-red emitting QDs by controlling the size and uniformity under iodide-rich conditions. Subsequently, vacancy defects and insulating ligands are cleared through introducing acid. Then this surface-cleaning process induces ligand exchange to further inhibit the nonradiative recombination and improve the electrical property of QDs. These QDs show a pure-red photoluminescence (PL) at 635 nm with the PL quantum yield (PLQY) of 99%. Finally, PeLEDs, which utilize these QDs, demonstrate a pure-red electroluminescence (EL) peak at 638 nm with a maximum external quantum efficiency (EQE) of 26.0% and an excellent half-lifetime (T-50) of 490 min at an original luminance of 102 cd/m(2).

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GB/T 7714 Ren, Ke , Hu, Jingcong , Bi, Chenghao et al. Strongly-Confined CsPbI3 Quantum Dots by Surface Cleaning-Induced Ligand Exchange for Spectrally Stable Pure-Red Light-Emitting Diodes with Efficiency Exceeding 26% [J]. | ACS MATERIALS LETTERS , 2024 , 6 (9) : 4115-4123 .
MLA Ren, Ke et al. "Strongly-Confined CsPbI3 Quantum Dots by Surface Cleaning-Induced Ligand Exchange for Spectrally Stable Pure-Red Light-Emitting Diodes with Efficiency Exceeding 26%" . | ACS MATERIALS LETTERS 6 . 9 (2024) : 4115-4123 .
APA Ren, Ke , Hu, Jingcong , Bi, Chenghao , Wei, Shibo , Wang, Xingyu , de Leeuw, Nora H. et al. Strongly-Confined CsPbI3 Quantum Dots by Surface Cleaning-Induced Ligand Exchange for Spectrally Stable Pure-Red Light-Emitting Diodes with Efficiency Exceeding 26% . | ACS MATERIALS LETTERS , 2024 , 6 (9) , 4115-4123 .
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High-Efficiency Pure-Red CsPbI3 Quantum Dot Light-Emitting Diodes Enabled by Strongly Electrostatic Potential Solvent and Sequential Ligand Post-treatment Process SCIE
期刊论文 | 2024 , 24 (15) , 4571-4579 | NANO LETTERS
WoS CC Cited Count: 2
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Abstract :

Efficient pure-red emission light-emitting diodes (LEDs) are essential for high-definition displays, yet achieving pure-red emission is hindered by challenges like phase segregation and spectral instability when using halide mixing. Additionally, strongly confined quantum dots (QDs) produced through traditional hot-injection methods face byproduct contamination due to poor solubility of metal halide salts in the solvent octadecene (ODE) at low temperatures. Herein, we introduced a novel method using a benzene-series strongly electrostatic potential solvent instead of ODE to prevent PbI2 intermediates and promote their dissolution into [PbI3](-). Increasing methyl groups on benzene yields precisely sized (4.4 +/- 0.1 nm) CsPbI3 QDs with exceptional properties: a narrow 630 nm PL peak with photoluminescence quantum yield (PLQY) of 97%. Sequential ligand post-treatment optimizes optical and electrical performance of QDs. PeLEDs based on optimized QDs achieve pure-red EL (CIE: 0.700, 0.290) approaching Rec. 2020 standards, with an EQE of 25.2% and T-50 of 120 min at initial luminance of 107 cd/m(2).

Keyword :

CsPbI3 quantum dots CsPbI3 quantum dots strongly confined strongly confined light-emitting diodes light-emitting diodes pure-red pure-red sequential ligand post-treatment sequential ligand post-treatment

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GB/T 7714 Hu, Jingcong , Bi, Chenghao , Ren, Ke et al. High-Efficiency Pure-Red CsPbI3 Quantum Dot Light-Emitting Diodes Enabled by Strongly Electrostatic Potential Solvent and Sequential Ligand Post-treatment Process [J]. | NANO LETTERS , 2024 , 24 (15) : 4571-4579 .
MLA Hu, Jingcong et al. "High-Efficiency Pure-Red CsPbI3 Quantum Dot Light-Emitting Diodes Enabled by Strongly Electrostatic Potential Solvent and Sequential Ligand Post-treatment Process" . | NANO LETTERS 24 . 15 (2024) : 4571-4579 .
APA Hu, Jingcong , Bi, Chenghao , Ren, Ke , Zhang, Xuetao , Wang, Weiqiang , Ma, Sai et al. High-Efficiency Pure-Red CsPbI3 Quantum Dot Light-Emitting Diodes Enabled by Strongly Electrostatic Potential Solvent and Sequential Ligand Post-treatment Process . | NANO LETTERS , 2024 , 24 (15) , 4571-4579 .
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Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production SCIE
期刊论文 | 2023 , 338 | APPLIED CATALYSIS B-ENVIRONMENTAL
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Electrochemical production of hydrogen peroxide (H2O2) is a sustainable and environmentally benign process. The electrochemical oxygen reduction process (ORR) via a two electron pathway (2e- ORR) offers a practical method for on-site H2O2 generation. As an earth-abundant catalyst, the cobalt-nitrogen coordinated systems integrated into the carbon matrix (Co-NC) has caused wide attention for its high activity in 2e- ORR. Even though most of the reported Co-NC catalysts have classical planar Co-N4 coordination, axial coordination engineering has recently emerged as an effective way to control the active sites in the axial direction by using different coordination ligands. The structure-function link between the Co-N configuration of non-planar coordination and 2e- ORR activity is, however, not fully understood. An axial-N coordinated Co-N5 motif embedded in hierarchically porous graphite-3R carbon (Co-N5C) was effectively synthesized using a template-sacrificing method. The Co-N5C has a high selectivity for 2e- ORR and a high H2O2 molar production rate of up to 6.78 mol peroxide/ gcatalyst/h in acidic media, both of which are better than its Co-N4 counterpart. DFT analyses demonstrate that axial-N ligands regulated the d-band center of the Co atom in the Co-N5C catalyst, inducing a shift in & UDelta;G*OOH near the Sabatier volcano plot's peak (& UDelta;G*OOH = 4.22 eV). This optimized the binding of the *OOH intermediate and then enhanced the protonation of *OOH to produce H2O2 more efficiently.

Keyword :

Template-sacrificing strategy Template-sacrificing strategy Hydrogen peroxide Hydrogen peroxide ORR ORR Active site density Active site density Axial-N Axial-N

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GB/T 7714 Yan, Lina , Wang, Chao , Wang, Yueshuai et al. Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 338 .
MLA Yan, Lina et al. "Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production" . | APPLIED CATALYSIS B-ENVIRONMENTAL 338 (2023) .
APA Yan, Lina , Wang, Chao , Wang, Yueshuai , Wang, Yahui , Wang, Zhaozhao , Zheng, Lirong et al. Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 338 .
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使役环境下钙钛矿光伏器件失稳机理研究
会议论文 | 2023 | 第十届新型太阳能材料科学与技术学术研讨会
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全面了解钙钛矿太阳能电池(PSC)及发光二极管(LED)的微结构衰变机理,对于发展高效稳定的钙钛矿光伏器件至关重要。前期工作中,通过发展先进电子显微学表征技术方法[1],我们针对钙钛矿太阳能电池在光、湿以及加热条件下的微结构演变过程,以及偏压加载下钙钛矿发光二极管的衰减机理进行了系统研究。研究结果表明,光照条件下,有机无机杂化钙钛矿薄膜会向金属铅Pb~0进行转变,在此过程中非晶相PbI_(2-x)在Pb~0表面形成壳层,对于有机无机杂化钙钛矿的降解过程至关重要~([2])。对于PSC器件而言,光照过程中金属电极如Au元素会向电子传输层与钙钛矿的界面处发生迁移,其对太阳能电池器件的光照稳定性扮演者重要的角色~([3,4])。在湿度条件下,有机无机杂化钙钛矿表面的有机封端和无机Pb-I封端,会造成其薄膜降解路径的差异~([1])。而加热条件下,电子传输层内部的氧元素会逐渐扩散至钙钛矿层,其对薄膜以及器件的热稳定性演化起着决定性作用~([5])。除上述研究外,我们还研究了偏压条件下无机CsPbI_3钙钛矿量子点及发光器件的降解路径,尤其揭示了表面卤素空位对其性能和稳定性降解路径的决定性影响~([6])。

Keyword :

钙钛矿 钙钛矿 光伏器件 光伏器件 结构与性能 结构与性能 稳定性 稳定性

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GB/T 7714 卢岳 . 使役环境下钙钛矿光伏器件失稳机理研究 [C] //第十届新型太阳能材料科学与技术学术研讨会论文集 . 2023 .
MLA 卢岳 . "使役环境下钙钛矿光伏器件失稳机理研究" 第十届新型太阳能材料科学与技术学术研讨会论文集 . (2023) .
APA 卢岳 . 使役环境下钙钛矿光伏器件失稳机理研究 第十届新型太阳能材料科学与技术学术研讨会论文集 . (2023) .
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电化学及光化学液体环境透射电子显微镜技术在能源催化研究领域的应用
期刊论文 | 2023 , (10) , 1126-1140 | 北京工业大学学报
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电化学及光化学液体环境透射电子显微镜技术由于能够对固-液相界面进行直接实时动态观测,近年来在能源催化机理研究领域的机理研究得到了应用。首先,对液体环境透射电子显微镜中引入电信号和光信号的平台设计方案进行了归纳总结;其次,对这项技术在电催化产氢、二氧化碳还原以及光催化产氢这几类典型的能源催化体系中的应用进行了分类介绍和成果总结;最后,针对这项技术的局限性进行了分析,提出了解决方案并在此基础上对其未来的发展方向进行了展望。电化学及光化学液体环境透射电子显微镜技术在为各类催化反应的机理研究提供有力的技术支持的同时,其分辨率问题以及电子束与材料的相互作用等方面所带来的假象应当引起研究人员的重视。

Keyword :

光催化 光催化 电催化 电催化 原位 原位 能源材料 能源材料 液体环境 液体环境 透射电子显微镜 透射电子显微镜

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GB/T 7714 王越帅 , 黄国裕 , 沈志桐 et al. 电化学及光化学液体环境透射电子显微镜技术在能源催化研究领域的应用 [J]. | 北京工业大学学报 , 2023 , (10) : 1126-1140 .
MLA 王越帅 et al. "电化学及光化学液体环境透射电子显微镜技术在能源催化研究领域的应用" . | 北京工业大学学报 10 (2023) : 1126-1140 .
APA 王越帅 , 黄国裕 , 沈志桐 , 卢岳 , 隋曼龄 . 电化学及光化学液体环境透射电子显微镜技术在能源催化研究领域的应用 . | 北京工业大学学报 , 2023 , (10) , 1126-1140 .
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Ferroelectricity in layered bismuth oxide down to 1 nanometer SCIE
期刊论文 | 2023 , 379 (6638) , 1218-1224 | SCIENCE
WoS CC Cited Count: 33
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Atomic-scale ferroelectrics are of great interest for high-density electronics, particularly field-effect transistors, low-power logic, and nonvolatile memories. We devised a film with a layered structure of bismuth oxide that can stabilize the ferroelectric state down to 1 nanometer through samarium bondage. This film can be grown on a variety of substrates with a cost-effective chemical solution deposition. We observed a standard ferroelectric hysteresis loop down to a thickness of similar to 1 nanometer. The thin films with thicknesses that range from 1 to 4.56 nanometers possess a relatively large remanent polarization from 17 to 50 microcoulombs per square centimeter. We verified the structure with first-principles calculations, which also pointed to the material being a lone pair-driven ferroelectric material. The structure design of the ultrathin ferroelectric films has great potential for the manufacturing of atomicscale electronic devices.

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GB/T 7714 Yang, Qianqian , Hu, Jingcong , Fang, Yue-Wen et al. Ferroelectricity in layered bismuth oxide down to 1 nanometer [J]. | SCIENCE , 2023 , 379 (6638) : 1218-1224 .
MLA Yang, Qianqian et al. "Ferroelectricity in layered bismuth oxide down to 1 nanometer" . | SCIENCE 379 . 6638 (2023) : 1218-1224 .
APA Yang, Qianqian , Hu, Jingcong , Fang, Yue-Wen , Jia, Yueyang , Yang, Rui , Deng, Shiqing et al. Ferroelectricity in layered bismuth oxide down to 1 nanometer . | SCIENCE , 2023 , 379 (6638) , 1218-1224 .
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Cation vacancy activating surface neighboring sites for efficient CO2 photoreduction on Bi4Ti3O12 nanosheets SCIE
期刊论文 | 2022 , 10 (38) , 20396-20401 | JOURNAL OF MATERIALS CHEMISTRY A
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Inefficient charge separation and insufficient surface catalytic sites remain the main impediment in developing highly efficient and selective catalysts for CO2 photoreduction. Surface defects are effective, but their function is always constrained within the defect location. Herein, a desirable surface cation vacancy strategy is implemented to solve the above obstacles over Bi4Ti3O12 nanosheets. The surface Ti vacancy (V-Ti) creates an atomic-level charge transfer channel on the surface of Bi4Ti3O12, allowing a rapid transfer of photon-generated electrons from the V-Ti site of neighboring Ti and O atoms to CO2 molecules. More importantly, V-Ti activates neighboring Ti and O atoms, which allows them a stronger ability for enhancing CO2 adsorption and conversion. Thus, a convenient and swift charge transfer channel and activated near surface region are formed on the surface of Bi4Ti3O12, profoundly boosting the CO2 reduction process, as evidenced by experimental and theoretical results collectively. Without any sacrificial agents or cocatalysts, Bi4Ti3O12 with an optimal V-Ti concentration exhibits an outstanding CO production rate of 15.17 mu mol g(-1) h(-1), nearly 5 times higher than that of pristine Bi4Ti3O12. This work unfolds a new function of surface cation vacancies to substantially enhance CO2 photoreduction.

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GB/T 7714 Liu, Lizhen , Hu, Jingcong , Lei, Ben et al. Cation vacancy activating surface neighboring sites for efficient CO2 photoreduction on Bi4Ti3O12 nanosheets [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2022 , 10 (38) : 20396-20401 .
MLA Liu, Lizhen et al. "Cation vacancy activating surface neighboring sites for efficient CO2 photoreduction on Bi4Ti3O12 nanosheets" . | JOURNAL OF MATERIALS CHEMISTRY A 10 . 38 (2022) : 20396-20401 .
APA Liu, Lizhen , Hu, Jingcong , Lei, Ben , Huang, Hongwei , Lu, Yue . Cation vacancy activating surface neighboring sites for efficient CO2 photoreduction on Bi4Ti3O12 nanosheets . | JOURNAL OF MATERIALS CHEMISTRY A , 2022 , 10 (38) , 20396-20401 .
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A High-Performance In-Memory Photodetector Realized by Charge Storage in a van der Waals MISFET SCIE
期刊论文 | 2022 , 34 (10) | ADVANCED MATERIALS
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The emerging data-intensive applications in optoelectronics are driving innovation toward the fused integration of sensing, memory, and computing to break through the restrictions of the von Neumann architecture. However, the present photodetectors with only optoelectronic conversion functions cannot satisfy the growing demands of the multifunctions required in single devices. Here, a novel route for the integration of non-volatile memory into a photodetector is proposed, with a WSe2/h-BN van der Waals heterostructure on a Si/SiO2 substrate to realize in-memory photodetection. This photodetector exhibits an ultrahigh readout photocurrent of 3.4 mu A and photoresponsivity of 337.8 A W-1 in the solar-blind wavelength region, together with an extended retention time of more than 10 years. Furthermore, the charge-storage-based non-volatile mechanism of h-BN/SiO2 is successfully proven through a novel analysis of in situ optoelectronic electron energy-loss spectroscopy. These results represent a leap forward to future applications and insightful mechanisms of in-memory photodetection.

Keyword :

non-volatile photodetection non-volatile photodetection charge-storage effect charge-storage effect 2D materials 2D materials van der Waals heterostructures van der Waals heterostructures in-memory photodetectors in-memory photodetectors

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GB/T 7714 Li, Songyu , Zhang, Zeyu , Chen, Xiaoqing et al. A High-Performance In-Memory Photodetector Realized by Charge Storage in a van der Waals MISFET [J]. | ADVANCED MATERIALS , 2022 , 34 (10) .
MLA Li, Songyu et al. "A High-Performance In-Memory Photodetector Realized by Charge Storage in a van der Waals MISFET" . | ADVANCED MATERIALS 34 . 10 (2022) .
APA Li, Songyu , Zhang, Zeyu , Chen, Xiaoqing , Deng, Wenjie , Lu, Yue , Sui, Manling et al. A High-Performance In-Memory Photodetector Realized by Charge Storage in a van der Waals MISFET . | ADVANCED MATERIALS , 2022 , 34 (10) .
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