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Function-reversible facets enabling SrTiO nanocrystals for improved photocatalytic hydrogen evolution

《能源前沿（英文）》 doi: 10.1007/s11708-023-0894-4

摘要： It has been widely reported that, for faceted nanocrystals, the two adjacent facets with different band levels contribute to promoted charge separation, and provide active sites for photocatalytic reduction and oxidation reaction, respectively. In such cases, only one family of facets can be used for photocatalytic hydrogen evolution. Herein, by using SrTiO3 nanocrystals enclosed by {023} and {001} facets as a model photocatalyst, this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all facets. The photo-deposition experiment of CdS provided direct evidence to demonstrate that the {023} facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles, together with the {001} facets. Thus, the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen, in contrast to those SrTiO3 nanocrystals with only {001} facets deposited by Pt nanoparticles via a photo-deposition method.

关键词： SrTiO3 nanocrystals     crystal facets     photocatalysis     hydrogen evolution    

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Design and synthesis of ZnCoO/CdS for substantially improved photocatalytic hydrogen production

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 606-616 doi: 10.1007/s11705-022-2233-4

摘要： In this study, the hydrogen evolution performance of CdS nanorods is improved using ZnCo2O4. ZnCo2O4 nanospheres are synthesized using the hydrothermal and calcination methods, and CdS nanorods are synthesized using the solvothermal method. From the perspective of morphology, numerous CdS nanorods are anchored on the ZnCo2O4 microspheres. According to the experimental results of photocatalytic hydrogen evolution, the final hydrogen evolution capacity of 7417.5 μmol∙g–1∙h–1 is slightly more than two times that of the single CdS, which proves the feasibility of our study. Through various characterization methods, it is proved that the composite sample has suitable optoelectronic properties. In addition, ZnCo2O4 itself exhibits good conductivity and low impedance, which shortens the charge-transfer path. Overall, the introduction of ZnCo2O4 expands the adsorption range of light and improves the performance of photocatalytic hydrogen evolution. This design can provide reference for developing high-efficiency photocatalysts.

关键词： ZnCo2O4 nanosphere     CdS nanorods     photocatalytic hydrogen evolution    

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Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1566-z

摘要：

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method.

关键词： Dual-functional photocatalysts     Oxygen-doped MoS2/ZnIn2S4     H2 evolution     Organic pollutant    

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Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

《能源前沿（英文）》 2022年 第16卷 第5期   页码 734-746 doi: 10.1007/s11708-022-0840-x

摘要： This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal–organic framework (MOF)-based systems toward the photocatalytic hydrogen evolution (PHE) reaction through specific strategies: tailoring the photocatalytic activity of bare MOFs and guest@MOF composites, formation of heterojunctions based on MOFs and various photocatalysts, and inorganic photocatalysts derived from MOFs. According to the data reported in this mini-review, the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units (SBUs). Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view, many of these studies relate this activity to the physicochemical and catalytic properties of MOFs. However, they did not consider the interactions between the components of the photocatalytic material. This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE. A thorough review and comparison of the results established that metal–nanoparticle@MOF composites have weak van der Waals forces between components, whereas heterostructures only interact with MOFs at the surface of bare materials. Regarding material derivatives from MOFs, we found that pyrolysis destroyed some beneficial properties of MOFs for PHE. Thus, we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.

关键词： metal–organic frameworks (MOFs)     photocatalytic hydrogen evolution     MOF heterojunctions     materials derived from MOFs     bandgap     recombination    

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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Roles of various Ni species on TiO

Xiaoping CHEN, Jihai XIONG, Jinming SHI, Song XIA, Shuanglin GUI, Wenfeng SHANGGUAN

《能源前沿（英文）》 2019年 第13卷 第4期   页码 684-690 doi: 10.1007/s11708-018-0585-8

摘要： Low-cost nickels can be used as cocatalyst to improve the performance of photocatalysts, which may be promising materials applied in the field of photocatalytic water splitting. In this study, different nickel species Ni, Ni(OH) , NiO, NiO , and NiS are used to modified titanium dioxide (P25) to investigate their roles on the photocatalytic hydrogen evolution activities. UV-visible, X-ray diffraction (XRD), Brunner-Emmet-Teller (BET) measurements, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) analysis etc. are employed to characterize the physical and chemical properties of catalysts. The results indicate that all the nickel species can improve the photocatalytic hydrogen production activity of P25. The P25 modified with NiO and NiS has more superior photocatalytic hydrogen evolution activities than those modified with other nickel species. The reason for this is that NiO and NiS can form p-n junctions with P25 respectively. In addition, NiO can be selectively deposited on the active sites of P25 via the photodeposition method and NiS is beneficial for H reacting with photo-excited electrons.

关键词： nickel species     TiO2     photocatalytic hydrogen evolution    

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Recent advances of hydrogen production through particulate semiconductor photocatalytic overall water

《能源前沿（英文）》 2022年 第16卷 第1期   页码 49-63 doi: 10.1007/s11708-022-0817-9

摘要： Solar energy-driven photocatalytic water splitting has been investigated for decades to produce clean and renewable green hydrogen. In this paper, the cutting-edge research within the overall water splitting system is summarized from the one-step photocatalytic overall water splitting (POWS) system to the two-step system and the cocatalysts research in this field. In addition, the photocatalytic reaction engineering study is also reviewed which is crucial for future scale-up. This mini-review provides a picture of survey of recent progress of relevant overall water splitting system, with particular attention paid to material system and mechanistic breakthroughs, and highlights the challenge and opportunity of the current system.

关键词： photocatalysis     overall water splitting     hydrogen    

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Factors affecting photocatalytic performance through the evolution of the properties due to the phase

《能源前沿（英文）》 2022年 第16卷 第3期   页码 471-482 doi: 10.1007/s11708-021-0778-4

摘要： The phase transition process of a photocatalytic system from NaBiO3·2H2O to BiO2–x has been investigated to understand the important factors that affect photocatalytic performance in a composite system. It is found that a proper amount of BiO2–x on the surface of NaBiO3·2H2O could effectively suppress the electron/hole recombination and increase the exposed reactive sites for photocatalytic reaction. A fully covered BiO2–x on NaBiO3·2H2O results in a dramatical decrease of photocatalytic degradation of dye. An over long hydrothermal process can result in BiO2–x with reduced oxygen vacancies, which degrades the photocatalytic activity. Furthermore, the photocatalytic reduction ability of CO2 conversion has been investigated, indicating that the surface activity to different reactants also directly affects the catalytic performance. The investigation of the gradient phase transition process presents a clear guidance to construct a desired photocatalytic system, in addition to selecting gradient materials with suitable bandgap structure and a morphology with different fraction and distribution of each component. The defect evolution of each component during construction of a composite is also an important factor that should be optimized and considered in making a composite to achieve high photocatalytic efficiency.

关键词： composite construction     distribution     BiO2–x     evolution of defects    

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Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 473-480 doi: 10.1007/s11705-018-1724-9

摘要：

The polypyrrole(PPy)@NiCo hybrid nanotube arrays have been successfully fabricated as a high performance electrocatalyst for hydrogen evolution reaction (HER) in alkaline solution. The strong electronic interactions between PPy and NiCo alloy are confirmed by X-ray photoelectron spectroscopy and Raman spectra. Because these interations can remarkably reduce the apparent activation energy (Ea) for HER and enhance the turnover frequency of catalysts, the electrocatalytic performance of PPy@NiCo hybrid nanotube arrays are significantly improved. The electrochemical tests show that the PPy@NiCo hybrid catalysts exhibit a low overpotential of ~186 mV at 10.0 mA·cm−2 and a small tafel slope of 88.6 mV·deg−1 for HER in the alkaline solution. The PPy@NiCo hybrid nanotubes also exhibit high catalytic activity and high stability for HER.

关键词： NiCo alloy     polypyrrole     hybrid nanotube     electrocatalyst     hydrogen evolution reaction    

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NiS heterostructure grown on nickel foam as efficient and durable self-supported electrocatalysts for hydrogenevolution reaction

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 437-448 doi: 10.1007/s11705-022-2228-1

摘要： High-performance and ultra-durable electrocatalysts are vital for hydrogen evolution reaction (HER) during water splitting. Herein, by one-pot solvothermal method, MoOx/Ni3S2 spheres comprising Ni3S2 nanoparticles inside and oxygen-deficient amorphous MoOx outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoOx/Ni3S2/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoOx/Ni3S2/NF-11 exhibits the best HER performance, requiring an extremely low overpotential of 76 mV to achieve the current density of 10 mA∙cm‒2 (η10 = 76 mV) and an ultra-small Tafel slope of 46 mV∙dec‒1 in 0.5 mol∙L‒1 H2SO4. More importantly, the catalyst shows prominent high catalytic stability for HER (> 100 h). The acid-resistant MoOx wraps the inside Ni3S2/NF to ensure the high stability of the catalyst under acidic conditions. Density functional theory calculations confirm that the existing oxygen vacancy and MoOx/Ni3S2 heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆GH*|) over Mo sites, which act as main active sites. The heterostructure effectively decreases the formation energy of O vacancy, leading to surface reconstruction of the catalyst, further improving HER performance. The MoOx/Ni3S2/NF is promising to serve as a highly effective and durable electrocatalyst toward HER.

关键词： molybdenum oxides     oxygen vacancies     heterostructure     electrocatalysts     hydrogen evolution reaction    

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Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

《能源前沿（英文）》 2021年 第15卷 第3期   页码 656-666 doi: 10.1007/s11708-021-0765-9

摘要： In recent years, defect-engineered Zr-based UiO-66 metal-organic frameworks (UiO-66(Zr) metal-organic frameworks (MOFs)) have shown huge advantages in catalytic, functional materials, adsorption, and other fields due to their large surface areas, well-ordered porous structures, and flexible tailorability. It is extremely challenging to introduce defect sites in the synthesis of MOFs to regulate the physicochemical properties of materials such as (energy band structure, pore structure, etc.) to obtain an excellent performance. This paper reviews the recent research results of synthesis methods, characterization technologies, and application fields of defect-engineered UiO-66(Zr) MOFs materials in order to provide new insights to synthesize high-performance UiO-66(Zr) MOFs materials and promote the development of UiO-66(Zr) in various fields.

关键词： defect engineering     metal-organic frameworks     UiO-66     photocatalysis    

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Theoretical study on flow and radiation in tubular solar photocatalytic reactor

《能源前沿（英文）》 2021年 第15卷 第3期   页码 687-699 doi: 10.1007/s11708-021-0773-9

摘要： In this paper, based on the mixture flow model, an optimized six-flux model is first established and applied to the tubular solar photocatalytic reactor. Parameters influencing photocatalyst distribution and radiation distribution at the reactor outlet, viz. catalyst concentration and circulation speed, are also analyzed. It is found that, at the outlet of the reactor, the optimized six-flux model has better performances (the energy increase by 1900% and 284%, respectively) with a higher catalyst concentration (triple) and a lower speed (one third).

关键词： photocatalytic hydrogen photoreactor     nume- rical simulation     solar energy     flow model     radiation model    

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In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytichydrogen production

《能源前沿（英文）》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要： Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词： photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

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High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

《能源前沿（英文）》 doi: 10.1007/s11708-023-0892-6

摘要： High entropy materials (HEMs) have developed rapidly in the field of electrocatalytic water-electrolysis for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unique properties. In particular, HEM catalysts are composed of many elements. Therefore, they have rich active sites and enhanced entropy stability relative to single atoms. In this paper, the preparation strategies and applications of HEM catalysts in electrochemical water-electrolysis are reviewed to explore the stabilization of HEMs and their catalytic mechanisms as well as their application in support green hydrogen production. First, the concept and four characteristics of HEMs are introduced based on entropy and composition. Then, synthetic strategies of HEM catalysts are systematically reviewed in terms of the categories of bottom-up and top-down. The application of HEMs as catalysts for electrochemical water-electrolysis in recent years is emphatically discussed, and the mechanisms of improving the performance of electrocatalysis is expounded by combining theoretical calculation technology and ex-situ/in situ characterization experiments. Finally, the application prospect of HEMs is proposed to conquer the challenges in HEM catalyst fabrications and applications.

关键词： high-entropy     electrocatalysis     synthetic methods     water-electrolysis     hydrogen and oxygen evolutions    

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A mini-review of ferrites-based photocatalyst on application of hydrogen production

《能源前沿（英文）》 2021年 第15卷 第3期   页码 621-630 doi: 10.1007/s11708-021-0761-0

摘要： Photocatalytic water splitting for hydrogen production is a promising strategy to produce renewable energy and decrease production cost. Spinel-ferrites are potential photocatalysts in photocatalytic reaction system due to their room temperature magnetization, the high thermal and chemical stability, narrow bandgap with broader visible light absorption, and proper conduction band energy level with strong oxidation activity for water or organic compounds. However, the fast recombination of the photoexcited electrons and holes is a critical drawback of ferrites. Therefore, the features of crystallinity, particle size, specific surface area, morphology, and band energy structure have been summarized and investigated to solve this issue. Moreover, composites construction with ferrites and the popular support of TiO2 or g-C3N4 are also summarized to illustrate the advanced improvement in photocatalytic hydrogen production. It has been shown that ferrites could induce the formation of metal ions impurity energy levels in TiO2, and the strong oxidation activity of ferrites could accelerate the oxidation reaction kinetics in both TiO2/ferrites and g-C3N4/ferrites systems. Furthermore, two representative reports of CaFe2O4/MgFe2O4 composite and ZnFe2O4/CdS composite are used to show the efficient heterojunction in a ferrite/ferrite composite and the ability of resistance to photo-corrosion, respectively.

关键词： photocatalyst     spinel-ferrite     composite     photocatalytic hydrogen production    

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标题 作者 时间 类型 操作

Function-reversible facets enabling SrTiO nanocrystals for improved photocatalytic hydrogen evolution

期刊论文

Design and synthesis of ZnCoO/CdS for substantially improved photocatalytic hydrogen production

期刊论文

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation

期刊论文

Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

期刊论文

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

Roles of various Ni species on TiO

Xiaoping CHEN, Jihai XIONG, Jinming SHI, Song XIA, Shuanglin GUI, Wenfeng SHANGGUAN

期刊论文

Recent advances of hydrogen production through particulate semiconductor photocatalytic overall water

期刊论文

Factors affecting photocatalytic performance through the evolution of the properties due to the phase

期刊论文

Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

期刊论文

NiS heterostructure grown on nickel foam as efficient and durable self-supported electrocatalysts for hydrogenevolution reaction

期刊论文

Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

期刊论文

Theoretical study on flow and radiation in tubular solar photocatalytic reactor

期刊论文

In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytichydrogen production

期刊论文

High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

期刊论文

A mini-review of ferrites-based photocatalyst on application of hydrogen production

期刊论文