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DALTON TRANSACTIONS · 2025 ·Vol. 54 ·期 8 ·3467-3477 · IF 3.3

TiO2/CoOx heterostructure decorated MIL-100(Fe) by atomic layer deposition for enhanced photocatalytic oxygen production

Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li

Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.

CAS / MDL: 7439-89-6
研究领域: 材料科学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Substrate-dependent ALD of Cux on TiO2 and its performance in photocatalytic CO2 reduction

Mu Liu,Liren Zheng,Xiaolei Bao,Zeyan Wang,Peng Wang,Yuanyuan Liu,Hefeng Cheng,Ying Dai,Baibiao Huang,Zhaoke Zheng

Atomic layer deposition (ALD) technique has been proved to be an efficient method to synthesize or modify catalyst. In this study, Cu was loaded on different TiO 2 substrates, pristine TiO 2 and black TiO 2 (denoted as H-TiO 2 ) to achieve better CO 2 photocatalytic reduction performance. Both TiO 2 @Cu and H-TiO 2 @Cu exhibited dramatic enhancement for CO and CH 4 production. The peculiar phenomenon of TiO 2 outperforming H-TiO 2 after ALD loading was further studied by a series of characterization methods. Even though H-TiO 2 showed superior performance for photocatalytic CO 2 reduction than TiO 2 , pristine TiO 2 loaded with more Cu 0/+ after ALD deposition surpassed the performance of H-TiO 2 @Cu which possessed less amount of Cu 0/+ and more Cu 2+ . Cu 0/+ is proved to be the crucial factor for CO 2 reduction and it is capable of overshadowing the influence of Ti 3+ and V o . These results indicate that not only will ALD technique significantly enhance the CO 2 reduction performance after Cu deposition, but the substrate employed for loading and the chemical state of loaded material will also influence the subsequent catalytic performance. In addition, our result provides additional experiment evidence for justifying the significance of Cu 0/+ in photocatalytic CO 2 reduction reaction.

CAS / MDL: 13463-67-7 16940-66-2
研究领域: 材料科学 · 环境科学
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Less is more: Enhancement of photocatalytic activity of g-C3N4 nanosheets by site-selective atomic layer deposition of TiO2

Peng Lv,Chongyang Zhao,Woo Jae Lee,Siping Huo,Se-Hun Kwon,Jun Fang,Yang Yang

Zero-dimensional/two-dimensional (0D/2D) TiO 2 /g-C 3 N 4 heterostructural photocatalysts were fabricated via ALD technique. TiO 2 nanoparticles were “site-selectively grown” on g-C 3 N 4 nanosheets and the surface modification induced band engineering of the composite photocatalysts. Thus, the redox properties of the photocatalysts were fine tuned. Under visible light , since only g-C 3 N 4 was excited, TiO 2 was acting as the electron transport channel in the optimized interfacial structures . They effectively suppressed the recombination and facilitated the transfer of photogenerated charges, improving the photocatalytic activity. When both the components were excited under UV–vis light, the dynamic equilibrium of the conduction band positions on these n–n type semiconductor heterojunctions led to the increased recombination rate of charges, decreasing the reactivity for H 2 evolution. However, the photocatalytic degradation of organic pollutants by these composite photocatalysts exhibited enhanced activities, resulting from the photogenerated holes on VB of TiO 2 which could promote oxidation of organic pollutants with strong oxidation potentials. Furthermore, TiO 2 /g-C 3 N 4 photocatalysts with limited numbers of deposition cycles exhibited optimal photocatalytic activity under visible light. In contrast, excessive deposition cycles on g-C 3 N 4 for TiO 2 /g-C 3 N 4 led to continuous film and increased thickness of TiO 2 , resulting in the attenuation of the reactivity. We verified this TiO 2 /g-C 3 N 4 photocatalysts with less mass-loading, but more enhanced photocatalytic activity.

CAS / MDL: 100-02-7
研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2017 · IF 6.035

Ceramic tubular nanofiltration membranes with tunable performances by atomic layer deposition and calcination

He Chen,Xiaojuan Jia,Mingjie Wei,Yong Wang

Ceramic nanofiltration (NF) membranes are of particular significance for molecular separations under harsh conditions. However, they are usually manufactured by the sol-gel process which frequently suffers from low efficiency and poor control in the membrane properties. Herein we demonstrate an efficient and more controllable strategy to produce ceramic tubular NF membranes based on atomic layer deposition (ALD). Tubular ceramic membranes with pore size of ~5   nm are used as the substrates, on which titanium alkoxide (titanicone) is ALD-deposited. Subsequent calcination in air degrades the organic moieties in titanicone, thus converting the dense layer of titanicone into a microporous layer of TiO 2 . This microporous TiO 2 layer serves as a thin separation layer delivering the NF size-sieving function. The thickness of the TiO 2 layer can be readily tuned by changing the ALD cycle numbers, and correspondingly the original substrate membranes are progressively tightened with rising ALD cycles, and the membrane with 300 cycles exhibits a molecular-weight-cut-off (MWCO) of ~680   Da and water permeability of 30   L   m −2   h −1   bar −1 . Such a water permeability is higher than many other ceramic tubular membranes with similar MWCOs because of the ultrathin nature of the microporous TiO 2 layer established by titanicone deposition and calcination.

CAS / MDL: 25322-68-3
研究领域: 材料科学 · 分离技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2020 · IF 3.573

Platinum Nanoparticle-Deposited Ti3C2Tx MXene for Hydrogen Evolution Reaction

Xiaobao Zhang,Baiyi Shao,Zemin Sun,Zhe Gao,Yong Qin,Ce Zhang,Fangming Cui,Xiaojing Yang

Nobel metal Pt composites show high catalytic activity for hydrogen evolution reaction (HER) but limited in application by high Pt contents and therefore the cost. Herein, a series of Pt nanoparticle (NP)-deposited 2D Ti3C2Tx MXenes were prepared by an atomic layer deposition (ALD) method with relatively low Pt contents (0.98–3.10 wt %) and showed excellent HER catalytic activity and stability. The electrochemical results indicated that the prepared catalysts showed the optimal HER activity as the ALD deposition cycle reached 40, with an overpotential of 67.8 mV approaching that of the commercial Pt/C catalyst (64.2 mV). The excellent behavior was attributed to the homogeneous dispersion of the Pt NPs and the good conductivity of the 2D Ti3C2Tx MXene supports.

CAS / MDL: 7664-39-3 2052-49-5
研究领域: 材料科学 · 电化学
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JOURNAL OF LUMINESCENCE · 2023 · IF 3.6

Optimum temperature of atomic layer deposition of alumina on CsPbBr3 quantum-dot for optical performance and environmental stability

Zijun Yan,Fangshun Ye,Liyue Xu,Xiao Yang,Shouqiang Lai,Shuli Wang,Yue Lin,Guolong Chen,Yijun Lu,Hao-Chung Kuo,Zhong Chen,Tingzhu Wu

Atomic layer deposition (ALD) plays a pivotal role in raising the long-term stability of perovskite quantum dot (PQD). The deposition temperature of excellent alumina film prepared by ALD is generally higher than 200 °C. In such a temperature environment, the lattice morphology of PQD is seriously damaged. In this work, to effectively protect PQD, the optimum temperature for depositing alumina on the surface of CsPbBr 3 PQD is investigated. The CsPbBr 3 PQD is deposited on a transparent glass substrate . Subsequently, an alumina layer is deposited on the surface of PQD via ALD at a deposition temperature of 40–120 °C. In our experiment, the significant degradation of PQD is observed when the deposition temperature of ALD is set to 80 °C and above. Lowering the deposition temperature can effectively improve the optical performance of PQD. The samples with alumina deposited at 75 °C show excellent stability after undergoing aging tests, and therefore 75 °C is considered the best ALD temperature. Besides, white light-emitting diode (W-LED) is produced by a method that a stack structure consisting of CsPbBr 3 coated via ALD at 75 °C and CdSe QD is excited using blue Micro-LED, and the color gamut of W-LED accounts for the wide area of 94.00% NTSC (1953) and 86.20% Rec.2020 displayed wide color gamut features. The experiment provides practical guidance for selecting the optimal deposition temperature for ALD-packaged PQD-based devices.

研究领域: 材料科学 · 光电技术
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Polyimide dielectrics sandwiched by large-bandgap Al2O3 for high-temperature energy storage

Hongmei Qin,Ziwei Li,Shiyu Qin,Yanda Jiang,Man Liu,Ling Zhou,Siyu Yu,Shan Wang,Chuanxi Xiong

High-temperature polymer dielectric capacitors are urgently needed in the new-generation electronic and electrical systems. Whereas, current commercial polymer represented by polyimide (PI) suffer from exponentially growing conduction loss at high temperatures and high electric fields, and hence extremely low discharged energy density and sharply declined charge-discharge efficiency. In this work, we developed superior Al 2 O 3 /PI/Al 2 O 3 sandwich films with drastically improved capacitive energy storage performance via atomic layer deposition (ALD) technology. Notably, resultant PI hybrid dielectrics deposited by 130 nm-thickness Al 2 O 3 (Al 2 O 3 /PI/Al 2 O 3 -130nm) exhibits the highest breakdown strength and the lowest leakage current density compared to pristine PI. Consequently, Al 2 O 3 /PI/Al 2 O 3 -130nm delivers a discharged energy density of 4.9 J/cm 3 at 25 °C and 3.3 J/cm 3 at 150 °C, as high as 2.7 times and 3.3 times respectively that of near PI film. Moreover, PI hybrid dielectrics can operate steadily under 200 MV/m and 150 °C during 10,000 cycle measurements. The excellent performance is mainly attributed to the improved barrier height of the electrode/PI interface endowed by deposited large-bandgap Al 2 O 3 .This work provides a scalable approach to enable excellent high-temperature energy storage performance of polymer dielectrics and promising to promote the application of PI for capacitive energy storage under harsh conditions.

研究领域: 材料科学 · 电气工程
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Atomic layer deposition precisely modified zeolite 13X: Physicochemical synergistic adsorption of space molecular contaminants

Yang Li,Wenjing Wei,Jiaqi Chen,Lijie Zu,Yan Zhou,Jinzhu Wu,Xiaohong Wu

In spaceflight applications, molecular contamination control has become one of the most challenging issues. Porous zeolites are a potent molecular adsorbent with advantages of efficient adsorption at low pressure and/or high temperature, high interaction with adsorbates, and superior durability in extreme environments. Herein, zeolite 13X pellets were selected for adsorption of stearyl alcohol (C 18 H 37 OH) as a target molecular contaminant. Considering the excellent hydrophilicity of the zeolite 13X which limits the adsorption of most hydrophobic organic molecules, modification of the zeolite 13X by deposition of TiO 2 via atomic layer deposition (ALD) technology was performed. Results show that ALD-grown TiO 2 not only improves hydrophobicity but also renders high activity, whilst retains the hierarchical pores of the zeolites. As a result, the as-prepared zeolite 13X@TiO 2 exhibits efficient adsorption toward trace stearyl alcohol under low pressure through the synergistic contribution of physisorption and chemisorption. Monte Carlo (MC) simulation, molecular dynamic (MD) and Density Functional Theory (DFT) calculations further discover that pore wall surfaces are primary adsorption sites for the physisorption while ALD-grown TiO 2 provides active sites for the chemisorption.

CAS / MDL: 112-92-5
研究领域: 材料科学 · 空间科学
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Advanced Materials Interfaces · 2022 ·Vol. 9 ·期 17 ·2200541 · IF 6.389

ZnO-Reinforced Thermal Regulating Microcapsules with Double-Layer Shell via Atomic Layer Deposition

Linfeng Li,Xi Wu,Xiaomeng Zhu,Yuanyuan Li,Liyi Zou,Xiuli Wang,Wenbin Li,Xiaomin Cheng

Conventional plain organic or inorganic shell for microcapsules has their own drawbacks, the organic shell has defects in thermal conductivity and stability; while the compactness and coverage of inorganic shell are not satisfactory. Herein, a novel approach to synthesis of organic–inorganic composite double-layer shell phase change microcapsule (DLSPCM) is proposed, which is achieved by forming inorganic outer shell on the surface of organic shell via atomic layer deposition (ALD). Taking the pristine microcapsule with paraffin core and melamine formaldehyde (MF) shell as an example, MF-ZnO composite double-layer shell (DLS) is formed in this paper. The melting enthalpy of DLSPCM obtained by 100 ALD cycles is 159.7 J g −1 , which is only 12.1 J g −1 lower than that of paraffin @ MF microcapsules (control sample), while the thermal conductivity of DLSPCM surges by 77.8%, and the thermal energy storage ability and thermal regulation performance are basically maintained. After 900 thermal cycles, the heat storage capacity of DLSPCM obtained by 100 ALD cycles decreased by only 3%. Besides, the photocatalytic performance and antibacterial activity of ZnO-reinforced DLSPCM are further confirmed. The successful design of DLSPCM via ALD is prospective for the encapsulation, modification, and reinforcement of phase change microcapsules.

CAS / MDL: 557-20-0 8002-74-2
研究领域: 材料科学 · 能源工程
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Solar RRL · 2021 ·Vol. 5 ·期 7 ·2100181 · IF 8.582

Defect Control for High-Efficiency Cu2ZnSn(S,Se)4 Solar Cells by Atomic Layer Deposition of Al2O3 on Precursor Film

Yali Sun,Pengfei Qiu,Siyu Wang,Hongling Guo,Rutao Meng,Xiaowei Zhou,Li Wu,Wei Yu,Jianping Ao,Yi Zhang

Cu 2 ZnSn(S,Se) 4 are emerging as promising photovoltaic materials due to their outstanding photoelectrical performances, benign grain boundaries, and Earth-abundant constituent elements. However, there are largely distributed cation-disordering defects and defect clusters, which lead to an increase in recombination and a large open-circuit voltage deficit and thus deteriorate device performance. Herein, defect control for a high-efficiency Cu 2 ZnSn(S,Se) 4 solar cell by atomic layer deposition of aluminum oxide (ALD-Al 2 O 3 ) on the precursor film is reporter. Cu Zn defects and Sn-related deep defects are largely suppressed because of the decrease in Sn 2+ and the increase in Sn 4+ in the film by ALD-Al 2 O 3 on the precursor are found, and the crystallinity of absorber layer is improved from a double-layer structure to a completely single-layer structure. Furthermore, the carrier lifetime and recombination in the bulk and interface are significantly improved for devices with ultrathin Al 2 O 3 . Using this approach, the conversion efficiency increases from 8.8% to 11.0% and the open-circuit voltage deficit decreases from 0.621 to 0.577 V. Herein, a deep understanding of the relationship between Al 2 O 3 incorporation and high-efficiency Cu 2 ZnSn(S,Se) 4 devices and a new direction for controlling defects to further improve the performance of kesterite solar cells are provided.

研究领域: 材料科学 · 太阳能电池研究
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Science China-Chemistry · 2021 ·Vol. 64 ·期 7 ·1088-1095 · IF 9.445

The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone

Zhai Liming,Zhang Bin,Liang Haojie,Wu Huibin,Yang Xinchun,Luo Gen,Zhao Shichao,Qin Yong

The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions. Because of the complex distribution of iron location on the support, the selectivity is always low. Here, we report a general strategy to selectively deposit highly-dispersed FeO x into the micropore of ZSM-5 by atomic layer deposition (ALD). The framework of ZSM-5 and the Brønsted acid sites are intact during ALD, and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5. Besides, more Fe-O-Si bonds are formed over FeO x /ZSM-5 with a low loading of Fe, while FeO x nanoparticles are generated at high Fe loading. They cannot be realized by the traditional solution method. The obtained FeO x /ZSM-5 catalysts perform high selectivity of cyclohexanone (92%–97%), and ALD cycle numbers of FeO x control the activity. Compared with the Fe nanoparticles, the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.

研究领域: 催化化学 · 材料科学
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Progress in Natural Science-Materials International · 2016 · IF 1.753

Atomic layer deposition on Pd nanocrystals for forming Pd-TiO2 interface toward enhanced CO oxidation

Yu Bai,Chunlei Wang,Xingyi Zhou,Junling Lu,Yujie Xiong

Pd typically exhibits relatively low catalytic activity in CO oxidation, as CO is apt to be adsorbed on Pd to poison the surface for O 2 activation. In this Letter, we report that this limitation can be overcome by integrating Pd with TiO 2 . The TiO 2 was coated on Pd nanocubes with a controllable thickness using atomic layer deposition (ALD) method. Given the different work functions of TiO 2 and Pd, the electrons in TiO 2 semiconductor will flow toward Pd. With the electron density increased on Pd, the adsorption of CO to Pd will be weakened while the oxygen activation can be facilitated. Meanwhile, the interface-confined sites at Pd-TiO 2 may further enhance the oxygen activation. As the species adsorption and activation are strongly correlated with electron density, the performance of Pd-TiO 2 in CO oxidation turns out to depend on the TiO 2 thickness, which determines the number of transferred electrons, within a certain range (<1.8   nm). This work provides a new strategy for enhancing catalytic performance through tailoring charge densities in hybrid catalysts.

CAS / MDL: 919-30-2 10025-98-6
研究领域: 材料科学 · 催化化学
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