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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Designed 2D/2D F-doped TiO2@ZnIn2S4 heterojunction for efficient photo-utilization hydrogen generation

Shumail Farhan,Asif Hassan Raza,Long Li,Songyu Yang,Yan Wu

Comprehending the catalytic reaction implementation for heterostructure photocatalysts is crucial by scrutinizing the spatial separation and transfer process of photoexcited charges at nanoscale junctions. Herein, we fabricated the F-doped TiO 2 /ZnIn 2 S 4 -based S-scheme heterostructure using a direct liquid-assembly method. The optimum hydrogen evolution rate (HER) of ∼ 1.58 mmol g –1 h –1 was acquired for 30-F 3 T@ZIS, which was about 15 and 2 times superior to the pristine F-doped TiO 2 and ZnIn 2 S 4 , respectively. The interaction between F-doped TiO 2 and ZnIn 2 S 4 facilitated the charge transfer from ZIS to F 3 T which was confirmed through XPS. UV–vis spectroscopy and Mott–Schottky validated that F-doped TiO 2 and ZnIn 2 S 4 retain the suitable energy band alignment for the S-scheme heterostructure. In situ, KPFM and EPR analysis revealed that F-doped TiO 2 and ZnIn 2 S 4 possess a spontaneous photoelectrochemical response, and their junction significantly improves the internal electric field by separating photoexcited charge carriers. This work provides a conclusive experimental and theoretical validation for an internal electric field and charge flow direction in non-noble-metal-based heterostructure photocatalysts.

研究领域: 材料科学 · 催化化学
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Journal of Physical Chemistry C · 2024 · IF 3.3

Preparation of 3D/2D ZnIn2S4/Porphyrin(Cu)-COF Type II Heterojunction: An In-Depth Insight into Interfacial Charge Transfer for Efficient Light-to-Hydrogen Conversion

Yu Xia,Guofang Huang,Yan Fan,Xiaolong Zhao,Lei Wang,Jingwei Huang,Houde She,Qizhao Wang

Semiconductor heterojunctions could accelerate carrier separation and transfer for improving light-to-hydrogen (LTH) conversion efficiency. However, the lack of tight and efficient interfacial charge cross in three-dimensional semiconductor-based heterojunctions limits their practical application and the relevant profound understanding of the interfacial charge delivery. In this work, porphyrin (Cu)-based COF with a highly conjugated structure was deposited onto three-dimensional (3D) ZnIn2S4 by a facile solvothermal method to prepare a 3D/2D ZnIn2S4@CuP–Ph COF heterojunction. The content-optimized ZnIn2S4@CuP–Ph COF composite showed an excellent LTH conversion rate of up to 2667.94 μmol g–1 h–1, about 13.5 times higher than that of pristine ZnIn2S4. The significantly meliorated photocatalytic performance is attributed to the synergistically functioning contributors, that is, the fast interfacial charge transfer and the augmented light capturing capability after integration. Also, the work function results by DFT calculation reveals that the electrons of CuP–Ph COF (Φ = 4.41 eV) transfer from the interface electron delivery channels of the two components to ZIS (Φ = 7.03 eV) until the Fermi level of the two components reaches equilibrium. This moment, the work function of ZnIn2S4@CuP–Ph COF (Φ = 6.50 eV) lies between the two components, and an electron accumulation region is formed on the side of ZIS. Additionally, the free-energy barriers of hydrogen evolution dominated by ZnIn2S4@CuP–Ph COF (0.0955 eV) is much lower than that of ZnIn2S4 (0.1256 eV). This study possesses certain guiding significance for the design of organic–inorganic heterojunction photocatalysts for efficient LTH conversion.

研究领域: 材料科学 · 能源科学 · 化学工程
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Nano Energy · 2018 · IF 13.12

Hierarchical CdS/m-TiO2/G ternary photocatalyst for highly active visible light-induced hydrogen production from water splitting with high stability

Yi Lu,Xiu Cheng,Ge Tian,Heng Zhao,Li He,Jie Hu,Si-Ming Wu,Ying Dong,Gang-Gang Chang,Silvia Lenaerts,Stéphane Siffert,Gustaaf Van Tendeloo,Zhao-Fei Li,Ling-Ling Xu,Xiao-Yu Yang,Bao-Lian Su

Hierarchical semiconductors are the most important photocatalysts , especially for visible light-induced hydrogen production from water splitting. We demonstrate herein a hierarchical electrostatic assembly approach to hierarchical CdS/m-TiO 2 /G ternary photocatalyst, which exhibits high photoactivity and excellent photostability (more than twice the activity of pure CdS while 82% of initial photoactivity remained after 15 recycles during 80 h irradiation). The ternary nanojunction effect of the photocatalyst has been investigated from orbitals hybrid, bonding energy to atom-stress distortion and nano-interface fusion. And a coherent separation mechanism of charge carriers in the ternary system has been proposed at an atomic/nanoscale. This work offers a promising way to inhibit the photocorrosion of CdS and, more importantly, provide new insights for the design of ternary nanostructured photocatalysts with an ideal heterojunction .

研究领域: 材料科学 · 能源科学 · 纳米技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Construction of ZnO/Zn3In2S6/Pt with integrated S-scheme/Schottky heterojunctions for boosting photocatalytic hydrogen evolution and bisphenol a degradation

Lifang Yang,Jiangju Si,Liang Liang,Yunfei Wang,Li Zhu,Zizhong Zhang

Photocatalytic water splitting has been identified as a promising solution to tackle the current environmental and energy crisis in the world. However, the challenge of this green technology is the inefficient separation and utilization of photogenerated electron-hole pairs in photocatalysts. To overcome this challenge in one system, a ternary ZnO/Zn 3 In 2 S 6 /Pt material was prepared as a photocatalyst using a stepwise hydrothermal process and in-situ photoreduction deposition. The integrated S-scheme/Schottky heterojunction in the constructed ZnO/Zn 3 In 2 S 6 /Pt photocatalyst enabled it to exhibit efficient photoexcited charge separation/transfer. The evolved H 2 reached up to 3.5 mmol g -1 h - 1 . Meanwhile, the ternary composite possessed a high cyclic stability against photo-corrosion under irradiation. Practically, the ZnO/Zn 3 In 2 S 6 /Pt photocatalyst also showed great potential for H 2 evolution while simultaneously degrading organic contaminants like bisphenol A. It is hoped in this work that the incorporation of Schottky junctions and S-scheme heterostructures in the construction of photocatalysts would lead to accelerated electron transfer and high photoinduced electron-hole pair separation, respectively, to synergistically enhance the performance of photocatalysts.

研究领域: 材料科学 · 环境科学 · 能源科学
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Journal of the Taiwan Institute of Chemical Engineers · 2023 · IF 5.7

Bandgap-energy-adjustable noble-metal-free MoS2-ZnxCd1−xS for highly efficient H2 production under visible-light

Linjuan Wang,Mingpu Kou,Julie Tournet,Siva Karuturi,Ling Zan

Background Recognized for its high calorific value, clean and non-polluting properties, hydrogen is considered to be one of the most attractive solutions to the impending energy crisis. Photocatalytic water splitting has been widely investigated for its promise to produce hydrogen in a sustainable, environmentally friendly and low-cost approach. In pursuit of high photocatalytic efficiency, multiple strategies haven been explored such as doping, co-catalyst modification and heterojunction construction realizing promising improvements. Methods We synthesized CdS doped with Zn ions and modified with MoS 2 as co-catalyst to form Zn x Cd 1− x S solid solution and MoS 2 -Zn 0.25 Cd 0.75 S heterojunction using a simple one-step hydrothermal method. The synthesized catalyst was used water splitting under visible light irradiation. The structural and morphological characteristics of these materials, along with their photocatalytic mechanisms, were investigated using multiple techniques such as SEM, TEM, XPS, PL, etc. Findings The photocatalyst consisting of 0.9 wt.% MoS 2 -Zn 0.25 Cd 0.75 S achieved a production rate of 6276 μmol h −1  g −1 , which is 17.4 times higher than that of pure CdS and 1.6 times higher than that of Zn 0.25 Cd 0.75 S. The composite also demonstrated a high apparent quantum yield of 11.1 % at 420 nm. The mechanism of the water splitting process, revealed through various techniques, introduces novel pathways for crafting high-efficiency photocatalysts with an internal electron-hole separation heterostructure.

CAS / MDL: 7631-95-0
研究领域: 材料科学 · 能源科学
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Advanced Energy Materials · 2024 · IF 24.4

Revolutionary Energy Harvesting: Gravity-Driven Piezocatalysts for Sustainable Hydrogen Production in MoS2@Mo2CTx Systems

Hsun-Yen Lin,Jyh Ming Wu

Hydrogen (H 2 ) is mainly produced using steam methane reforming, electrolysis, and gasification, which require external energy and special catalysts. A new catalyst by combining MoS 2 nanoflowers (NFs) with metal carbide/nitride nanosheets (Mo 2 CTx MXene) to create a nanosheet bending moment. The MoS 2 @Mo 2 CT x heterostructures achieve a production rate of 1164.8 µmol g −1 h −1 under an application of mechanical force, 4.01 and 3.06 times higher than Mo 2 CTx and MoS 2 alone, due to enhanced charge transfer from MoS 2 's piezoelectricity and Mo 2 CT x 's conductivity. This study introduces a pioneering methodology that harnesses gravitational energy as a continuous mechanical force, simulated using a peristaltic pump, to drive the piezocatalytic hydrogen evolution reaction (HER), achieving a notable hydrogen production rate of 454.1 µmol g −1 over 24 hours and demonstrating a sustained capability for hydrogen generation. The theoretical calculation results validate the piezoelectric potential in water-flow-pressure triggered HER systems. The piezocatalytic HER system, assuming powered by the Hoover Dam, will produce 290.9 kmoles of hydrogen per ton daily, equivalent to utilizing 19 150 kWh of energy in the electrocatalytic system. The simulated gravity-driven water flow using MoS 2 @Mo 2 CT x piezocatalysts for H 2 generation demonstrates superior efficiency by eliminating common thermal energy conversion losses, marking a significant breakthrough in sustainable hydrogen production technologies.

研究领域: 材料科学 · 可再生能源 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Near-infrared, eco-friendly ZnAgInSe quantum dots-sensitized graphene oxide-TiO2 hybrid photoanode for high performance photoelectrochemical hydrogen generation

Zhihang Long,Xin Tong,Cheng Liu,Ali Imran Channa,Rui Wang,Xin Li,Feng Lin,Alberto Vomiero,Zhiming M. Wang

Colloidal semiconductor quantum dots (QDs) are promising building-blocks for the manufacture of cost-effective photoelectrochemical (PEC) cells towards efficient solar-to-hydrogen conversion. Nevertheless, the state-of-the-art QDs-based PEC systems still suffer from the frequent utilization of highly toxic elements in QDs (Cd and Pb), hindering their future practical applications and potential commercialization. Here, we report a PEC device fabricated using eco-friendly, near-infrared (NIR) ZnAgInSe (ZAISe) QDs and hybrid TiO 2 /graphene oxide (GO) film. Based on the synergistic effect of QD’s broad light absorption and excellent charge extraction/transport properties of TiO 2 /GO film, as-assembled QDs-photoanode exhibits an outstanding saturated photocurrent density of ~6.7 mA/cm 2 with good stability under standard 1 sun illumination. The introduction of functional GO can lead to the reduced charge transfer resistance, suppressed charge recombination, and enhanced electron transport within the QDs-TiO 2 photoanodes. The results offer a facile and effective method to enhance the performance of environmentally friendly QDs-based PEC devices and shed light on the development of low-cost, “green” and high-efficiency solar-to-hydrogen conversion system.

CAS / MDL: 1314-23-4
研究领域: 材料科学 · 能源科学
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Energies · 2024 ·Vol. 17 ·期 3 ·646 · IF 3

Expectations for the Role of Hydrogen and Its Derivatives in Different Sectors through Analysis of the Four Energy Scenarios: IEA-STEPS, IEA-NZE, IRENA-PES, and IRENA-1.5°C

Osama A. Marzouk

Recently, worldwide, the attention being paid to hydrogen and its derivatives as alternative carbon-free (or low-carbon) options for the electricity sector, the transport sector, and the industry sector has increased. Several projects in the field of low-emission hydrogen production (particularly electrolysis-based green hydrogen) have either been constructed or analyzed for their feasibility. Despite the great ambitions announced by some nations with respect to becoming hubs for hydrogen production and export, some quantification of the levels at which hydrogen and its derived products are expected to penetrate the global energy system and its various demand sectors would be useful in order to judge the practicality and likelihood of these ambitions and future targets. The current study aims to summarize some of the expectations of the level at which hydrogen and its derivatives could spread into the global economy, under two possible future scenarios. The first future scenario corresponds to a business-as-usual (BAU) pathway, where the world proceeds with the same existing policies and targets related to emissions and low-carbon energy transition. This forms a lower bound for the level of the role of hydrogen and its penetration into the global energy system. The second future scenario corresponds to an emission-conscious pathway, where governments cooperate to implement the changes necessary to decarbonize the economy by 2050 in order to achieve net-zero emissions of carbon dioxide (carbon neutrality), and thus limit the rise in the global mean surface temperature to 1.5 °C by 2100 (compared to pre-industrial periods). This forms an upper bound for the level of the role of hydrogen and its penetration into the global energy system. The study utilizes the latest release of the annual comprehensive report WEO (World Energy Outlook—edition year 2023, the 26th edition) of the IEA (International Energy Agency), as well as the latest release of the annual comprehensive report WETO (World Energy Transitions Outlook—edition year 2023, the third edition) of the IRENA (International Renewable Energy Agency). For the IEA-WEO report, the business-as-usual situation is STEPS (Stated “Energy” Policies Scenario), and the emissions-conscious situation is NZE (Net-Zero Emissions by 2050). For the IRENA-WETO report, the business-as-usual situation is the PES (Planned Energy Scenario), and the emissions-conscious situation is the 1.5°C scenario. Through the results presented here, it becomes possible to infer a realistic range for the production and utilization of hydrogen and its derivatives in 2030 and 2050. In addition, the study enables the divergence between the models used in WEO and WETO to be estimated, by identifying the different predictions for similar variables under similar conditions. The study covers miscellaneous variables related to energy and emissions other than hydrogen, which are helpful in establishing a good view of how the world may look in 2030 and 2050. Some barriers (such as the uncompetitive levelized cost of electrolysis-based green hydrogen) and drivers (such as the German H2Global initiative) for the hydrogen economy are also discussed. The study finds that the large-scale utilization of hydrogen or its derivatives as a source of energy is highly uncertain, and it may be reached slowly, given more than two decades to mature. Despite this, electrolysis-based green hydrogen is expected to dominate the global hydrogen economy, with the annual global production of electrolysis-based green hydrogen expected to increase from 0 million tonnes in 2021 to between 22 million tonnes and 327 million tonnes (with electrolyzer capacity exceeding 5 terawatts) in 2050, depending on the commitment of policymakers toward decarbonization and energy transitions.

研究领域: 能源研究 · 环境科学 · 政策分析
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Surfaces and Interfaces · 2025 · IF 6.3

Silver-modified Bi2WO6 nanosheets for efficient hydrogen production via piezo-photo-catalysis

Lujie Ruan,Honglin Zhou,Xiangyu Li,Yuxuan Wang,Pengfei Luo,Haixuan Wang,Jiangping Ma,Chaogang Ban,Xiaoxing Wang,Jiangjie Ye,Yajie Feng,Jili Yue,Li-Yong Gan,Xiaoyuan Zhou,Ji-Yan Dai

Addressing the growing demand for clean energy necessitates innovative approaches to enhance hydrogen production efficiency. Combining photo-catalysis and piezo-catalysis offers a synergistic strategy for energy conversion, yet the limited charge transfer and separation efficiency in pure Bi 2 WO 6 hinders its catalytic performance. Herein, by adopting Ag nanoparticles deposited on Bi 2 WO 6 nanosheets (Bi 2 WO 6 –2% Ag) as a paradigm, it is demonstrated that the incorporation of Ag significantly enhances charge separation and transfer via improved piezoelectric and electronic interactions. This modification not only boosts the piezoelectric coefficient by 1.78-fold but also promotes the generation of piezo-induced and photogenerated carriers. Consequently, Bi 2 WO 6 –2% Ag achieves a hydrogen yield of 14.3 mmol·g -1 ·h -1 under piezo-catalytic conditions, a 60.7% improvement compared to pristine Bi 2 WO 6 . Under combined piezo-photo-catalytic conditions, the hydrogen yield further increases to 30.9 mmol·g -1 ·h -1 . The enhanced performance is attributed to the synergistic effects of ultrasonic vibration and ultraviolet light, which induce band bending and polarization-driven charge migration, facilitating hydrogen production. This study provides valuable insights into the integration of noble metal deposition and piezo-photo-catalysis, opening a new pathway for the design of advanced catalysts for sustainable hydrogen energy solutions.

研究领域: 材料科学 · 能源化学
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Petroleum Science · 2024 · IF 6

Study on the mass transfer characteristics of hydrogen in heavy oil by a modified dynamic pressure step method

Tao Jiang,Fei Yu,Qian-Min Jiang,Yan-Xin Song,Qing-Feng Tan,Wu Su,Xu Yang,Zhen-Tao Chen,Chun-Ming Xu

The dissolved hydrogen, rather than gaseous hydrogen, plays a crucial role in the hydrogenation process. A thorough understanding of hydrogen dissolution is essential for optimizing the hydrogenation process. In this paper, the dynamic pressure step method was modified to reduce the temperature difference between the hydrogen and solution, from which the hydrogen solubility and volumetric liquid-side mass transfer coefficient ( k L a ) of the vacuum residue were obtained. It was discovered that temperature was the most critical factor in hydrogen dissolution, simultaneously enhancing both the hydrogen solubility and k L a . Pressure played a significant role in promoting hydrogen solubility, but had a relatively small impact on k L a . Stirring speed, although it enhanced k L a , did not affect hydrogen solubility. By normalizing the dissolution parameter, the results showed that the gas-liquid mass transfer rate decreased continuously during hydrogen dissolution and that the S D - t D curves after normalization were almost the same in all experimental conditions.

CAS / MDL: 544-76-3
研究领域: 化学工程 · 石油加工
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MATERIALS LETTERS · 2021 · IF 3.423

High piezo-photocatalytic efficiency of H2 production by CuS/ZnO nanostructure under solar and ultrasonic exposure

Tianming Zhao,Qi Wang,An Du

To alleviate the energy shortage and to improve the environmental problems, low-cost and highly efficient materials for H 2 production are of considerable importance. Here, we report a nanostructure from CuS/ZnO NWs on steel mesh via a two-step hydrothermal route for piezo-photocatalytic H 2 production. The CuS/ZnO exhibits an absorption band in visible and ultra-violet bands. Under solar and ultrasonic exposure, the CuS/ZnO NWs demonstrate great piezo-photocatalytic performance (140 μmol g −1  h −1 ). The working mechanism can be attributed to the piezo-photocatalytic effect that the photogenerated electrons and holes are driven along opposite directions by built-in electrical field, decreasing the recombination rate and producing H 2 . This H 2 production mechanism holds great promise for development novel clean fuel.

CAS / MDL: 1313-84-4
研究领域: 材料科学 · 能源科学 · 环境科学
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Light-Irradiated Thermal Energy-Promoted Selective Phenol Hydrogenation on Cellulose-Supported Palladium Catalyst with Green Hydrogen

Peijing Guo,Shaoyu Yuan,Chenyang Yu,Zhangyi Xiong,Yushan Yang,Jianlong Du,Yaguang Li,Yongjun Gao

The energy and environmental crises urge us to develop a green and sustainable catalytic strategy to achieve chemical transformation. Thus, light-irradiated thermal energy, green hydrogen generated from water electrolysis, and natural cellulose were combined into a catalytic system for phenol hydrogenation to cyclohexanone in this article. The cellulose containing abundant hydroxyl groups improves the catalytic activity of palladium nanoclusters supported on it and hinder the overhydrogenation of cyclohexanone to cyclohexanol. DFT calculations and control experiments demonstrate that the existence of glucose (the monomer of cellulose) on a Pd surface facilitates the dissociative adsorption of phenol on a catalyst and deactivates the hydrogenation of cyclohexanone to cyclohexanol, which further clarifies the higher catalytic activity and better selectivity of Cel-1Pd. More importantly, the selective hydrogenation of phenol to cyclohexanone can be conducted smoothly in a photothermal reactor under irradiation of a xenon lamp, effectively facilitating the benign conversion between light, thermal, and chemical energies.

CAS / MDL: 9004-34-6
研究领域: 化学工程 · 环境科学 · 材料科学
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