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Pt–Ba–Ce/γ-Al₂O₃ 催化剂，物理化学性质，NO_x存储和还原，NO_x 排放，H₂ 还原剂 1

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

《能源前沿（英文）》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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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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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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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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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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growth of NiSe nanocrystalline array on graphene for efficient hydrogen evolution reaction

《能源前沿（英文）》页码 595-600 doi: 10.1007/s11708-022-0827-7

摘要： Nickel selenide electrocatalysts for hydrogen evolution reaction (HER) with a high efficiency and a low-cost have a significant potential in the development of water splitting. However, the inferiority of the high overpotential and poor stability restricts their practical applications. Herein, a composite nanostructure consists of ultrasmall NiSe₂ nanocrystals embedded on graphene by microwave reaction is reported. The prepared NiSe₂/reduced graphite oxide (rGO) electrocatalyst exhibited a high HER activity with an overpotential of 158 mV at a current density of 10 mA/cm² and a corresponding moderate Tafel slope of 56 mV/dec in alkaline electrolyte. In addition, a high retention of electrochemical properties (approximately 100%) was demonstrated with an unchangeable microstructure after 100 h of continuous operation.

关键词： nickel selenide carbon materials nanoparticles hydrogen evolution reaction (HER) microwave reaction

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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 BiO_2–_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 BiO_2–_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 BiO_2–_x on NaBiO₃·2H₂O results in a dramatical decrease of photocatalytic degradation of dye. An over long hydrothermal process can result in BiO_2–_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 BiO_2–_x evolution of defects

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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）》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, MoO_x/Ni₃S₂ spheres comprising Ni₃S₂ nanoparticles inside and oxygen-deficient amorphous MoO_x outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoO_x/Ni₃S₂/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoO_x/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 MoO_x 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 MoO_x/Ni₃S₂ heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆G_H*|) 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 MoO_x/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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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 (E_a) 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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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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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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Persulfate-induced three coordinate nitrogen (N3C) vacancies in defective carbon nitride for enhanced photocatalyticH2O2 evolution

Wei Miao,Yijie Wang,Ying Liu,Hehe Qin,Chengcheng Chu,Shun Mao,

《工程（英文）》 doi: 10.1016/j.eng.2021.12.016

摘要： In-situ photocatalytic H2O2 production has been receiving increasing attention in recent years for sustainable H2O2 synthesis. Graphitic carbon nitride (g-C3N4) is regarded as one of the most promising semiconductor photocatalysts for H2O2 evolution. Introducing N defects in g-C3N4 has been proved to be an effective strategy to enhance photocatalytic activity. However, the photocatalytic mechanism of the N vacancies is ambiguous and different types of N vacancies in g-C3N4 may exhibit different effects on photocatalytic activity. Herein, we develop a facile sodium persulfate eutectic polymerization method to prepare the g-C3N4 with abundant three coordinate nitrogen (N3C) vacancies. This type of nitrogen vacancy has not been studied in g-C3N4 for photocatalytic H2O2 production. Our results showed that the introduction of N3C vacancies in the g-C3N4 successfully broadened the light absorption range, inhibited the photoexcited charge recombination with enhanced O2 adsorption to promote oxygen activation. The photocatalytic H2O2 evolution from the N3C-rich g-C3N4 is 4.5 times higher than that of the pristine g-C3N4. This study demonstrates a novel strategy to introduce N3C vacancies in g-C3N4, which offers a new method to develop active catalysts for photocatalytic H2O2 evolution.Graphical abstractDownload : Download high-res image (60KB)Download : Download full-size image

关键词： Carbon nitride N3 C vacancy Hydrogen peroxide evolution Photocatalysis Persulfate

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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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Z-scheme CdS/WO on a carbon cloth enabling effective hydrogen evolution

《能源前沿（英文）》 2021年第15卷第3期页码 678-686 doi: 10.1007/s11708-021-0768-6

摘要： Photocatalytic water splitting for hydrogen (H₂) generation is a potential strategy to solve the problem of energy crisis and environmental deterioration. However, powder-like photocatalysts are difficult to recycle, and the agglomeration of particles would affect the photocatalytic activity. Herein, a direct Z-scheme CdS/WO₃ composite photocatalyst was fabricated based on carbon cloth through a two-step process. With the support of carbon cloth, photocatalysts tend to grow uniformly for further applications. The experimental results showed that the H₂ yield of adding one piece of CdS/WO₃ composite material was 17.28 μmol/h, which was 5.5 times as compared to that of pure CdS-loaded carbon cloth material. A cycle experiment was conducted to verify the stability of the as-prepared material and the result demonstrated that the H₂ generation performance of CdS/WO₃ decreased slightly after 3 cycles. This work provides new ideas for the development of recyclable photocatalysts and has a positive significance for practical applications.

关键词： photocatalysis CdS/WO₃ carbon cloth Z-scheme hydrogen evolution

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标题作者时间类型操作

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

期刊论文

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

期刊论文

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

期刊论文

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

期刊论文

Recent advances of hydrogen production through particulate semiconductor photocatalytic overall water

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

growth of NiSe nanocrystalline array on graphene for efficient hydrogen evolution reaction

期刊论文

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

期刊论文

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

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

Theoretical study on flow and radiation in tubular solar photocatalytic reactor

期刊论文

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

期刊论文

Persulfate-induced three coordinate nitrogen (N3C) vacancies in defective carbon nitride for enhanced photocatalyticH2O2 evolution

Wei Miao,Yijie Wang,Ying Liu,Hehe Qin,Chengcheng Chu,Shun Mao,

期刊论文

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

期刊论文

Z-scheme CdS/WO on a carbon cloth enabling effective hydrogen evolution

期刊论文

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