INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2014
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IF 2.93
Jian Yu,Si-Liang Lei,Tong-Cai Chen,Jian Lan,Jian-Ping Zou,Lin-Hua Xin,Sheng-Lian Luo,Chak-Tong Au
A new strategy has been put forward to improve the performance of photocatalytic H 2 evolution of tantalate-based catalysts through designing solid solutions Bi 1− x In x TaO 4 combined with CdS, among which the solid solutions Bi 1− x In x TaO 4 ( x = 0, 0.1, 0.3, 0.5, 0.7, 0.9, and 1.0) were firstly synthesized by the citrate method using cheap and environment-friendly Ta 2 O 5 . The experimental results reveal that the Bi 0.5 In 0.5 TaO 4 solid solution shows the best photocatalytic performance among the Bi 1− x In x TaO 4 solid solutions. And in the absence of noble metals, the 30% CdS/Bi 0.5 In 0.5 TaO 4 (30CBITO) catalyst exhibits good photocatalytic hydrogen evolution from water splitting with a rate of H 2 production of 511.75 μmol h −1 g −1 under simulated sunlight irradiation. And the rate of hydrogen evolution does not markedly change for 60 h. Their compositions , structures and morphologies were characterized by UV–vis diffusion reflectance spectroscopy (DRS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HRTEM). A photocatalytic enhancement mechanism was put forward to elucidate the superior photocatalytic activity and long-term stability of the heterostructured CdS/Bi 0.5 In 0.5 TaO 4 composites.
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ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Yong Liu,Kai Yan,Jingdong Zhang
Graphitic carbon nitride (g-C3N4) is a new type of metal-free semiconducting material with promising applications in photocatalytic and photoelectrochemical (PEC) devices. In the present work, g-C3N4 coupled with CdS quantum dots (QDs) was synthesized and served as highly efficient photoactive species in a PEC sensor. The surface morphological analysis showed that CdS QDs with a size of ca. 4 nm were grafted on the surface of g-C3N4 with closely contacted interfaces. The UV–visible diffuse reflection spectra (DRS) indicated that the absorption of g-C3N4 in the visible region was enhanced by CdS QDs. As a result, g-C3N4–CdS nanocomposites demonstrated higher PEC activity as compared with either pristine g-C3N4 or CdS QDs. When g-C3N4–CdS nanocomposites were utilized as transducer and tetracycline (TET)-binding aptamer was immobilized as biorecognition element, a visible light-driven PEC aptasensing platform for TET determination was readily fabricated. The sensor showed a linear PEC response to TET in the concentration range from 10 to 250 nM with a detection limit (3S/N) of 5.3 nM. Thus, g-C3N4 sensitized with CdS QDs was successfully demonstrated as useful photoactive nanomaterials for developing a highly sensitive and selective PEC aptasensor.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2015
·
IF 2.999
Lin Tang,Yaocheng Deng,Guangming Zeng,Wei Hu,Jiajia Wang,Yaoyu Zhou,Jingjing Wang,Jing Tang,Wei Fang
This paper described a facile method for the design and utilization of three-dimensional TiO 2 branched nanorod arrays with CdS and Cu 2 S quantum dots co-sensitized photoelectrode for photoelectrochemical water splitting . CdS and Cu 2 S quantum dots were attached on the surface of TiO 2 BNRs by successive ionic layer adsorption and reaction (SILAR). The morphology and element composition of the fabricated samples were characterized by field emission scanning electron microscopy (FE-SEM), high resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), and the optical features were measured by UV–vis diffuse reflection spectroscopy (UV–vis DRS) and photocurrent density–voltage (I–V) curves. The photocurrent value can be significantly enhanced due to the introduction of CdS and Cu 2 S quantum dots on the TiO 2 BNRs surface. The 9 cycles of CdS and 6 cycles of Cu 2 S presented the best performance and reached a high photocurrent density to 13.65 mA at 0 V versus Ag/AgCl and hydrogen generation efficiency of 7.74% at −0.467 V versus Ag/AgCl. This enhancement can be attributed to the improved light absorption and the heterojunction formed between CdS and Cu 2 S, which can greatly promote the introduction and transportation of the photo electrons. This work provided a facile way for the synthesis of high performance photoelectrode for photoelectrochemical water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Gang Yu,Liping Liu,Chong Zhao,Shuaiqi Guo,Haibing Meng,Yongfa Zhu,Xian-Ming Zhang
Metal-organic frameworks (MOFs) as high-efficiency photocatalysts often face limitations due to the inadequate charge separation and sluggish charge transfer kinetics. Herein, we construct an interfacial linker coordinated heterostructure cadmium sulfide/zirconium-based metal–organic framework (CdS/NU-M) for high-efficiency photocatalytic H 2 evolution. The interfacial thiol coordination significantly narrows the energy difference between conduction band of NU-M and valence band of CdS, achieving a Z-scheme charge transfer channel in CdS/NU-M. As a result, a robust internal electric field is found in the formed Z-scheme heterojunction of CdS and NU-M, which is 20 times higher than that of NU-M. Thus, photogenerated charge carries are efficiently separated and transported to the surface, which induces CdS/NU-M with a 10-fold increase of photocatalytic H 2 evolution rate over the contrast photocatalyst, up to 84.3 mmol g −1 h −1 , prominently surpassing most of the reported MOFs and CdS-based photocatalysts. This work highlights the crucial role of interfacial linker coordination in enhancing charge separation and transfer, significantly improving the photocatalytic performance and providing an effective strategy for designing advanced photocatalysts and related technologies.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yanting Dou,Yu Gao,Bobo Bai,Jiqi Zheng,Xiufang Wang,Hongjiang Li,Yi Li,Qiuhui Bu,Dongling Ma,Fu Ding,Yaguang Sun,Zhenhe Xu
To improve the photocatalytic activities of photocatalysts, constructing heterojunction structures is considered as an effective measure. Herein, a series of the 1D (one dimensional)/2D (two dimensional) CdS/Ag-doped ZnIn 2 S 4 (denoted as CdS/Ag:ZIS) heterojunctions were constructed by growing 2D Ag:ZIS nanoplates on 1D CdS nanowires. Under visible light irradiation, the optimized CdS/Ag:ZIS shows H 2 production rate of as high as 2447.02 μmol g −1 h −1 , which has increased by 7.8 and 2.2 times compared to pure CdS and Ag:ZIS, respectively. Meanwhile, the degradation efficiency of methyl orange (MO) reaches 99.45% within 50 min. The enhanced photocatalytic activity is due to the improved absorption of visible light along with accelerated separation of photogenerated carriers, thanks to the formation of an intimate interface, suitable energy band alignment and abundant active sites. Furthermore, CdS/Ag:ZIS also exhibits high stability in both photocatalytic processes, with negligible decay over multiple photocatalytic cycles. Based on the results of density functional theory (DFT) and photoelectrochemical characterizations, a Z-scheme heterojunction is proposed, followed by in-depth studies of the charge transfer processes and the photocatalytic mechanisms.
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ACS Catalysis
·
2024
·
IF 11.3
Yuheng Ma,Yu Zhang,Guanshun Xie,Zhaohui Huang,Linfen Peng,Changqiang Yu,Xiuqiang Xie,Shuanglin Qu,Nan Zhang
Doping engineering has enabled the construction of homogeneous and abundant atomic-level catalytic sites for photocatalytic CO2 reduction with improved selectivity for the target product. However, little is known about the effect of the spatial position of the heteroatoms on the photocatalytic activity of the semiconductors toward CO2 reduction. Herein, uniform Cu doping into the bulk phase of hollow CdS cubes (HCC) and Cu doping onto the surface of HCC, denoted as Cu/HCC and HCC@Cu, respectively, are prepared by tuning the introduction order of Cu sources. Experimental analysis shows that the introduction of Cu by both methods can promote the separation and migration of photoinduced charge carriers in CdS. Notably, Cu doping onto the surface of CdS in HCC@Cu leads to much better proton reduction to H2 production performance but lower CO2 reduction efficiency as compared to bare CdS. In sharp contrast, Cu doping into the bulk phase of CdS enhances the CO2-to-CO conversion while mitigating H2 evolution. This should be ascribed to the smaller overpotential of Cu/HCC in the CO2 saturated system than that in the Ar system. In addition, doping Cu atoms into the bulk phase of CdS shifts the d band center of Cu/HCC upward to near the Fermi energy level, which promotes the adsorption and activation of CO2 on CdS. These results indicate that the photoelectrons with a prolonged lifetime in Cu/HCC preferably reduce CO2 molecules rather than protons. The density functional theory (DFT) calculation results show that the introduction of Cu heteroatoms can promote the desorption of CO*, and the adaptable sulfur vacancies (Vs) produced by in situ doping techniques can stimulate the formation of CO* intermediates, resulting in the high performance of photocatalytic CO2 reduction to CO. This work reveals the effect of different heteroatom doping locations on the catalytic activity and will provide a reference for the design of efficient photocatalysts with atomic-level fine structure.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Yudong Guo,Xiya Chen,Yuxin Liu,Zhenjun Chen,Peiyuan Guo,Dongxiang Luo,Menglong Zhang,Xiao Liu
In a dual-functional lignin valorization system, a harmonious oxidation and reduction rate is a prerequisite for high photocatalytic performance. Herein, an efficient and facile ligand manipulating strategy to balance the redox reaction process is exploited via decorating the surface of the CdS@ZnxCd1–xS@ZnS gradient-alloyed quantum dots with both inorganic ligands of hexafluorophosphate (PF6–) and organic ligands of mercaptopropionic acid (MPA). Inorganic ion ligands in this system provide a promotion for intermediator reduction reactions. By optimizing the ligand composition on the quantum dot surface, we achieve precise control over the extent of oxidation and reduction, enabling selective modification of reaction products; that is, the conversion rate of 2-phenoxy-1-phenylethanol reached 99%. Surface engineering by regulating the ligand type demonstrates that PF6– and thiocyanate (SCN–) inorganic ion ligands contribute significantly toward electron transfer, while MPA ligands have beneficial effects on the hole-transfer procedure, which is predominantly dependent on their steric hindrance, electrostatic action, and passivation effect. The present study offers insights into the development of efficient quantum dot photocatalysts for dual-functional biomass valorization through ligand design.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Ranfeng Li,Zhenhua Dai,Taiyu Huang,Qianqian Zhang,Xunfu Zhou,Zhongli Peng,Zuotao Liu,Yueping Fang
CdS with a visible light response and energy band location suitable for CO 2 photoreduction has received extensive attention. However, low product selectivity and photocatalytic efficiency limit its application. Here, NaBH 4 is used as a reducing agent to generate Cd metal on the surface of CdS nanorods in situ. This leads to the construction of a B-CdS/Cd metal cocatalyst/semiconductor structure. This configuration significantly enhanced the CdS's activity of photocatalytic CO 2 reduction. The Cd metal which is on the surface of CdS nanorods promoted the separation and transfer of photogenerated charges and increased both light photosensitivity and CO 2 adsorption capabilities. The improved B-CdS/Cd catalyst shows excellent CO 2 reduction capabilities by generating CO at a rate of 323.39 μmol g − 1 h − 1 , which is 2.01 times more than pure CdS, owing to the synergistic enhancements. Simultaneously, Cd acts as an active site inhibiting H 2 production during the CO 2 reduction reaction. This work demonstrates the potential of Cd metal as a metal cocatalyst in photocatalytic CO 2 reduction.
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Catalysts
·
2025
·Vol. 15
·期 1
·94
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IF 4
Fuhai Zhang,Jing Xiong,Xiaoxiao Yu,Lei Wang,Tongyu Wu,Zhendong Yu,Minmeng Tang,Haiyan Liu,Yanhong Chao,Wenshuai Zhu
As a promising member of the carbon nitride family, nitrogen-rich g-C3N5has attracted significant attention because of its excellent light absorption performance. Nevertheless, its practical application in photocatalytic CO2reduction is hindered by severe photogenerated charge recombination and limited CO2adsorption capacity. Constructing a heterojunction has emerged as an effective strategy to mitigate charge recombination, thereby enhancing the photocatalytic performance of the catalyst. Herein, a series of CdS/g-C3N5-X heterojunction catalysts were prepared via an in situ hydrothermal approach. The obtained heterojunction catalysts exhibited a novel coral reef-like morphology which facilitated the exposure of additional active sites, thereby enhancing the adsorption and activation of CO2. Moreover, studies have shown that CdS can be anchored to the surface of g-C3N5through C-S bonds, forming a built-in electric field at the interface, which accelerated the separation and transfer of photogenerated charges. Consequently, the resulting heterojunction materials demonstrated high efficiency in photocatalytic CO2reduction with H2O as a sacrificial agent. In particular, CdS/g-C3N5-0.2 exhibited the maximum photocatalytic performance up to 22.9 μmol·g−1·h−1, which was 6 times and 3 times that of unmodified g-C3N5and CdS, respectively. The results indicated that the increased active sites and enhanced charge separation of the Cd/g-C3N5-0.2 catalyst were the primary reasons for its improved photocatalytic CO2reduction performance. This work provides a novel heterojunction-based photocatalyst for efficient CO2photocatalytic reduction, offering insights into the preparation of high-performance photocatalysts for sustainable energy applications.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 10
·3036-3046
·
IF 6.1
Shiheng Liang,Liugang Wu,Yiming Wang,Yuqi Shao,Hongyuan Song,Ziliang Chen,Weiju Hao
The construction of high-efficiency long-stable catalytic electrodes for hydrogen by seawater splitting is a huge challenge in the field of green hydrogen generation. Herein, a matrix-type titanium dioxide nanorod (Ti/TiO2) is constructed on the titanium plate (Ti) by one-step oxidative etching, and a two-dimensional self-supporting electrode with good stability and “local photothermal effect” strategy is constructed as a self-supporting electrode by carbon quantum dots (CDs) “inserted” self-growing iron boron (CDs-FeBx@TiO2). Based on the microstructure regulated by CDs, the in situ growth of FeB with high conductivity and high authenticity activity, the effective separation of electron–hole pairs in the TiO2 structure is promoted, and efficient photothermal seawater electrolysis is realized. The performance of hydrogen/oxygen evolution reaction (HER/OER) and overall seawater splitting of the highly active CDs-FeBx@TiO2 electrode increased by 14.7%, 16.2% and 4.4% at 10 mA cm−2 in alkaline simulated seawater. The CDs-FeBx@TiO2 electrode remains durable for 70 days at 100 mA cm−2 and even at industrial current density, and the catalytic activity remained at 93.5%. This work provides a simple way for the preparation of catalytic electrodes with high activity and excellent stability and provides theoretical support for the practical application of high purity hydrogen from seawater.
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Molecular Catalysis
·
2025
·
IF 4.9
Jiaxin Song,Cheng Rao,Zeshu Zhang,Xiangguang Yang,Yibo Zhang
Photocatalytic reforming of plastics, involving converting plastics into valuable chemicals while producing hydrogen from water, is a promising green technology with sustainability potential. However, designing catalysts with optimized structures to further enhance efficiency remained a major challenge. In this study, a series of CdS Quantum dots (QDs) with different sulfur defect concentrations were synthesized by a one-step solvothermal method by adjusting the type of sulfur precursors. In the absence of co-catalysts, the optimal CdS-NS photocatalyst achieved reforming of polyethylene terephthalate (PET) into formate with 870 μmol g −1 h −1 and acetate esters with 90 μmol g −1 h −1 , while the hydrogen production rate reached 1771 μmol g −1 h −1 . EPR spectra and other analyses confirmed the presence of abundant sulfur defects in the prepared CdS QDs and further demonstrated that the concentration of sulfur defects was closely related to photocatalytic performance. Suitable sulfur defects effectively modulated the electronic and band structure of CdS QDs, enhanced the oxidation capacity of photogenerated holes, reduced the recombination rate of charge carriers, and ultimately improved photocatalytic activity. This work provided an effective approach for designing efficient photocatalysts for the high-value recycling of plastic waste to achieve carbon neutrality.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2025
·Vol. 64
·期 27
·e202425601
·
IF 16.9
Yuemei Li,Shi-Yu Guo,Hongfei Gu,Bingyu Wang,Peiwu Su,Xiuming Zhang,Haoqing Zhang,Shuping Zhang,Fanzhi Yang,Jia Liu,Qing-An Chen,Jiatao Zhang
Visible light photoredox catalysis has become a rapidly emerging area owing to its potential of using sunlight to tame previously hard-to-harness radicals for organic synthesis. At present, such a blueprint faces a significant challenge, namely how to accomplish thermodynamically demanding reactions with sunlight encompassing a wide range of low-energy photons. Here, we report a new reaction framework to overcome this bottleneck through decoupling the thermodynamic limits of photoreduction from photoexcitation. This is fulfilled based on the construction of a heterogeneous photocatalyst Cu@CdS possessing in situ-formed surficial polysulfide species (including S 3 •− and S 4 2− ), which can efficiently harvest solar energy via plasmonic absorption of Cu while manifest sufficient redox potential for activating inert aryl bromides/chlorides enacted by excited polysulfides. We demonstrate that this designed material composes a potent photoredox catalyst for efficient aryl cross-coupling, borylation, hydrogenation, as well as Birch-type dearomatization reactions, with good recyclability and stability. In particular, when exclusively using natural sunlight as an energy source, the product yield can still reach up to 90%. Our findings introduce a straightforward yet viable way to progress toward the century-long dream of leveraging natural sunlight to produce structurally complex organic molecules, just like plants on Earth. Graphical Chemists have long aspired to construct complex organic compounds the way that plants do by harnessing natural sunlight as an energy source. This study presents an advancement toward this goal via synergistic exploitation of the plasmonic absorption of Cu and the unique redox potentials of excited polysulfide species (S 3 •− and S 4 2− ) on semiconductor surfaces to decouple the thermodynamic limits of photoreduction from photoexcitation.
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