JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xiaoyan Zhang,Wenkang Ni,Xuanyu Yue,Zhijie Wang,Zizhong Zhang,Ke Wang,Wenxin Dai,Xianzhi Fu
Converting CO 2 into CO, CH 4 , and other hydrocarbons using solar energy presents a viable approach for addressing energy shortages. In this study, photocatalysts with S-deficient WO 3 /Zn 3 In 2 S 6 (WO 3 /V S -ZIS) S-scheme heterojunctions have been successfully synthesized. Under UV–vis light irradiation, 20 %WO 3 /V S -ZIS demonstrated significantly improved CO 2 reduction activity and CH 4 selectivity. Detailed characterization and density functional theory (DFT) calculations reveal that the enhanced performance is due to the synergistic optimization of the S-scheme heterojunction and sulfur vacancies (V S ) for CO 2 reduction. The presence of V S aids in the adsorption and activation of CO 2 and enhances the separation of charge carriers. The 2D/2D S-scheme heterostructure assembled with WO 3 nanosheets not only accelerates the migration and separation of photoexcited charge carriers but also improves the adsorption of H 2 O and the formation of V S , thereby increasing the adsorption and activation of CO 2 and facilitating the protonation of CO* to produce CH 4 . This study clarifies the synergistic effect of V S and S-scheme heterostructures in improving photocatalytic performance, offering valuable insights into the photoactivation process of CO 2 at V S in S-scheme heterojunctions.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Zewei Liao,Jincheng Liu,Yijun Luo,Wei Cai,Bingjie Li,Xiaoyan Xiang,Yanxiong Fang
Due to the higher susceptibility of alcohols and ketones to oxidation compared to alkanes, converting inert C-H bonds in alkanes into high value-added product KA oil with high selectivity is still a significant obstacle. In this study, flower-like microspheres of MoO 3-x , featuring aligned nanosheets and oxygen vacancies, were combined with nitrogen doped carbon dots (NCDs) to fabricate S-scheme heterojunctions of MoO 3-x -NCDs for boosting the photocatalytic efficiency in oxidizing cyclohexane. Because of the oxygen vacancies-triggered localized surface plasmon resonance (LSPR) and the S-scheme charge transfer mechanism, there was a significant improvement in the absorption of visible light and an enhancement in the efficiency of charge separation. The MoO 3-x -NCDs composites exhibited a notably improved catalytic performance in cyclohexane oxidation. The MoO 3-x -NCDs composite exhibited remarkable selectivity of KA oil in catalyzing cyclohexane oxidation under light exposure, attributed to the substantial increase in cyclohexane adsorption capacity. The highest cyclohexane transformation rate of 9.98 % was achieved by MoO 3-x -NCDs-2 composites with a MoO 3-x /NCDs ratio of 50:1, outperforming bare MoO 3-x by 1.81 times, while exhibiting a KA oil selectivity reaching 93.75 %. The mechanism of selective photocatalytic oxidation was explored using photoelectric examination, analysis of energy bands, and evaluation of active radicals. In this research, green photocatalysts were fabricated through the utilization of NCDs, enabling efficient conversion and selective oxidation of cyclohexane in gentle environments. This innovative approach holds great potential for advancing the field of photocatalysis.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Small
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2024
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IF 13
Shikai Wang,Dong Zhang,Xipeng Pu,Lizhi Zhang,Dafeng Zhang,Jizhou Jiang
Herein, guided by the results of density functional theory prediction, the study rationally designs a hollow core–shell FeNi 2 S 4 @ZnIn 2 S 4 (FNS@ZIS) Step-scheme (S-scheme) heterojunction for photocatalytic H 2 evolution with photothermal-assisted. The hollow FNS spheres offered substrate for coating the ZIS nanosheets, which can inhibit ZIS nanosheets from agglomerating into pellet, enrich the active site, increase specific surfaces, and raise the light absorption. Notably, due to its excellent photothermal properties, FNS core generated heat unceasingly inside under visible-light irradiation and effectively prevent the heat loss of the reaction system, which increased the local temperature of photocatalysts and thus accelerated the charge migration. In addition, the S-scheme heterojunction construction via in situ growth has a tight interface, which can facilitate the separation and transfer of carriers and achieve high redox potential. Owning to the distinctive construction, the hollow core–shell FNS@ZIS S-scheme heterojunction show extraordinary stability and photocatalytic H 2 evolution rate with 7.7 mmol h −1 g −1 , which is ≈15.2-fold than pristine ZIS. Based on the double evidence of theoretical predictions and experimental confirmations, the photothermal effect and electron transfer mechanism of this innovative material are investigated in depth by the following infrared thermography technology and deep DFT calculations.
研究领域:
材料科学
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能源化学
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理论计算
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产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
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2025
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IF 6.7
Yang Yu,Lichao Xu,Kaiyuan Xu,Yan Li,Hao Chen,Dongxu Zhang,Yuanzi Chen,Yue Liu,Wenyue Qi
The construction of S-scheme heterojunctions has drawn widespread attention within the photocatalysis field due to their capacity for efficient separation of photogenerated carriers, leading to excellent photo-oxidation-reduction performance. Herein, a novel S-scheme loofah biochar/MoS 2 /g-C 3 N 4 (LB/MS/CN) heterojunction was successfully constructed by ultrasonication in 50 % ethyl alcohol and heat treatment in N 2 atmosphere. Degradation experiments showed that the 5 % LB/MS/CN ternary photocatalyst had optimal photocatalytic efficiency (96.4 %) for the degradation of rhodamine B (RhB), and the reaction rate (k) of this photocatalyst (0.05420 min −1 ) was 5.4 times that of unmodified CN (0.01001 min −1 ). Ultraviolet-visible diffuse reflectance spectra, Mott-Schottky, and free radical trapping experiments suggested that the photogenerated carriers in LB/MS/CN were transferred through the S-scheme structure. Consequently, the co-catalytic action of LB and the synergistic impact of the heterojunction structure between CN and MS led to a reduced photogenerated carrier recombination rate. Furthermore, LB/MS/CN had outstanding stability and the capacity to maintain RhB degradation performance under various environmental conditions (H 2 PO 4 − , NO 3 − , SO 4 2− , HCO 3 − , NaCl, humic acid (HA), and real water), showing good promise for practical applications. Thus, this work provides a possible strategy for purifying wastewater under visible light.
研究领域:
环境科学
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材料科学
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光催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Tao Guo,Danjun Mao,Xiufeng Lu,Wenhao Ma,Heyun Fu,Huan He,Cheng Sun,Shourong Zheng,Zhifeng Jiang,Xiaolei Qu
Inadequate contact interface, lack of direct electron-transfer paths and low substrate affinity are considered as the main obstacle inhibiting the heterostructure activity for the sustainable photosynthesis of value-added fine chemicals. Herein, a novel 0D/2D Step-scheme (S-scheme) α-Fe 2 O 3 /PbBiO 2 I (FO/PBOI) composite with abundant interface Fe O bonds were initially synthesized via an in-situ growth approach. The created built-in field as a powerful driving force, efficiently steering the migration of photogenerated electrons. The interfacial Fe O bonds act as atomic-level transfer highway, lowering charge transfer energy barrier between the interfaces and further accelerating the S-scheme spatial charge separation. Moreover, the Fe O bonds bridged FO/PBOI can effectively enhance the activation of O 2 and benzylamine, significantly reducing the dehydrogenation barrier for the rate-limiting C 6 H 5 CH 2 NH* intermediate. The optimized FO/PBOI exhibits remarkably improved catalytic activity and general applicability for the dehydrocoupling of primary amines to imines. This work offers an atomic-scale perspective on precise charge flow steering based on interface bond for advanced organic transformations.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2022
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IF 4.177
Yuyao Zhang,Yu Tian,Wen Chen,Min Zhou,Siyong Ou,Yueli Liu
The CO2 photoreduction process is becoming a promising strategy to solve the energy shortage problem and global warming in recent years. How to promote the separation of photoinduced carriers has attracted attention for the improvement of photocatalytic CO2 reduction. In the present work, an S-scheme heterojunction of Bismuthene/CsPbBr3 quantum dots (Bismuthene/CsPbBr3 QDs) is constructed as the photocatalyst for CO2 conversion. As a result, Bismuthene/CsPbBr3 QDs exhibit an optimal CH4 evolution rate of 43.1 μmol h–1 g–1 with 84.53% selectivity over CH4 under ultraviolet–vis light (UV–vis) irradiation. Construction of the S-scheme heterojunction with a narrow band gap semiconductor is the main factor for improving the photocatalytic performance, as the S-scheme heterojunction can suppress the recombination of photoinduced carriers and retain redox ability. The narrow band gap semiconductor Bismuthene can enhance light absorption abilities. This work probably provides some insights for the designing of heterojunction photocatalysts and the improvement of photocatalytic performance.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lijun Zhang,Zhiliang Jin,Noritatsu Tsubaki
As a crucial part of artificial photosynthesis, the design of the catalyst is important essential. Among them, the interface engineering between semiconductors and the construction of surface-active sites play a vital role in generating and transporting light-excited electrons, which can ultimately accelerate water decomposition. Therefore, the MoS 2 @MoO 3 step (S)-scheme heterojunction photocatalyst was prepared by in-situ partial sulfidation. The excellent interface engineering of MoS 2 @MoO 3 nanomaterials achieves a high surface reaction rate. The in-situ vulcanization strategy gradually corrodes from the outside to the inside. The introduction of sulfur atoms can replace oxygen atoms to build a sulfur-rich surface and generate molybdenum sulfide. The amount of thioacetamide is adjusted to control vulcanization and optimizing the experimental conditions, the best hydrogen production rate is 12416.8 µmol h −1 g −1 . An in-situ irradiation XPS experiments and DFT calculations provide a deeper understanding of the S-scheme electron transport mechanism in MoS 2 @MoO 3 . MoS 2 @MoO 3 interface interaction has penetrating electron channels and a strong interface interaction force, which effectively promotes the charge transfer between interfaces. This gradual surface vulcanization strategy provides new ideas for introducing synergistic surface-active sites and optimizing interface engineering photocatalyst projects.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Ya Xiong,Teng Liu,Xinyu Wang,Wendi Liu,Yanjun Xue,Xiaoli Zhang,Can Xiong,Jian Tian
Ultrathin CdS nanosheets (NSs) are intriguing in photocatalytic hydrogen evolution . Severe photo-corrosion and rapid recombination of electrons and holes, however, impair their applications. To solve this problem, a novel step-scheme (S-scheme) 2D CdS/W 18 O 49 heterostructure with strong interfacial interactions and large contact interface has been successfully designed. Due to the ultrathin structure of CdS, defect-rich W 18 O 49 NSs-assembled network, unique 2D heterostructure and state-of-the-art S-scheme mode, 40 wt% CdS/W 18 O 49 (CW40) shows a prominent photocatalytic H 2 production rate of 15.4 mmol g −1 h −1 . Besides, the apparent quantum efficiency of CW40 is up to 15.4 % under light at λ = 370 nm. Besides, the as-prepared CW40 can protect CdS from photo-corrosion, exhibiting outstanding stability over 24 h circular reaction. Our work provides an out-of-box solution to broaden the application potential of certain catalysts with inherent drawbacks and offers fresh insight into the design and preparation of highly-efficient 2D heterostructures for versatile applications.
研究领域:
材料科学
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能源化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Xinwei Zhang,Xiaotian Zhang,Rong Wang,Yijia Zhong,Kunting Li,Lei Xu,Huimin Feng
S-scheme heterojunction catalysts have attracted much attention due to their ability to effectively separate photo-generated electrons and holes while optimizing the redox ability of carriers. We have prepared an efficient visible-light catalytic PDPB/Ag–TiO 2 S-scheme heterojunction by in-situ synthesis methods . The catalysts were characterized for their structure, composition , morphology, and photoelectrochemical properties. The hydrogen production rate of PDPB/Ag–TiO 2 -2 was 1473.6 μmol/g/h. The results of SPV analysis showed that the spontaneous interfacial charge transfer from PDPB to Ag–TiO 2 in the contact interface region resulted in the presence of an internal electric field . This enhanced internal electric field effectively drove directional charge migration through the S-scheme mechanism, improving charge separation and utilization. The PDPB/Ag–TiO 2 -2 composites also maintained stable photocatalytic activity after running for four cycles. Overall, this study brings fresh preparation ideas for the conjugated polymer-TiO 2 composites with high photocatalytic efficiency.
研究领域:
材料科学
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能源化学
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光催化
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Zhihan Yu,Chen Guan,Xiaoyang Yue,Quanjun Xiang
Enhancing the carrier separation in graphitized carbon nitride (g-C 3 N 4 ) is advantageous for improving its photocatalytic activity. Herein, we propose a feasible method for preparing CN-C by thermal polymerization to gradually infiltrate carbon rings (C-rings) into the surface of crystalline carbon nitride (CN), enabling photogenerated electrons to be transferred rapidly between the CN inner layers and the CN/C outer layer. Successful penetration and distribution of carbon rings into carbon nitride were confirmed by secondary ion mass spectroscopy using ratio analysis of C and N elements at various depths of the prepared photocatalyst. Theoretical calculations indicated that CN and CN/C in the molecule generated different Fermi levels to form an S-scheme homojunction, establishing appropriate built-in electric fields and thus enabling interlayer charge migration. Moreover, the overlap of the conjugate plane of C-rings with carbon nitride led to the formation of photogenerated in-plane charge transfer tunnels. The two-electron transfer tunnels greatly improved the dissociation efficiency of photogenerated electrons. The prepared sample loaded with 3 wt% Pt as a co-catalyst for hydrogen production under visible light irradiation, and the prepared optimal sample CN-C showed a maximum quantum efficiency of 15.56% for photocatalytic H 2 evolution at 385 nm. This research introduces a new idea for constructing a directional transfer path for charge carriers in-plane and intralayer.
研究领域:
材料科学
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光催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yining Zhang,Mengyang Xu,Weiqiang Zhou,Xianghai Song,Xin Liu,Jisheng Zhang,Songtao Chen,Pengwei Huo
Step-scheme (S-scheme) heterojunctions can efficiently promote the separation of photogenerated carriers while maintaining the strong oxidation/reduction ability of photocatalysts; thus, research attention on S-scheme heterojunctions is increasing year by year. In this study, the S-scheme ZnO@ZnIn 2 S 4 (ZnO@ZIS) heterojunction was prepared successfully. Then, electron spin resonance (ESR) characterization was applied to prove the successful construction of the S-scheme heterojunction. Photoluminescence (PL), time-resolved photoluminescence (TRPL), and photoelectrochemical experiments have demonstrated efficient interfacial charge transport in ZnO@ZIS. Finally, the mechanism of CO 2 activation and electron transport was investigated by in situ Fourier transform infrared spectroscopy (FT-IR) and discrete Fourier transform (DFT) calculation analysis. The 40-ZnO@ZIS composite showed the best activity under light, and its CO and CH 4 yields reached 39.76 and 3.92 μmol∙g −1 ∙h −1 , respectively. This study provides a solution for optimizing the photocatalytic reduction activity of semiconductor photocatalysts by constructing S-scheme heterojunction materials to improve the CO 2 reduction capacity.
研究领域:
材料科学
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环境科学
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物理化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhiang Hou,Jinzhu Yue,Hao Chen,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Endocrine disrupting chemicals (EDCs) interfere with the normal secretion, transport and metabolism of human hormones, thus affecting neurological, reproductive and immune functions. Photocatalysis is regarded as a facile organic degradation technique. The construction of heterojunctions can modulate the reactive oxygen species and enhance the photocatalytic performance of semiconductors. However, poor contact interfaces still severely limit carrier separation and transfer. Herein, we have doped Co to modulate the band structure of Bi 2 O 2 CO 3 while facilitating the in situ growth of BiOI on its surface via shared Bi atoms. This approach led to the development of a 2D/2D Co-Bi 2 O 2 CO 3 /BiOI (Co-BOC/BiOI) S-scheme heterojunction characterized by atomically close contact interfaces. Furthermore, the photo-electrochemical characterization results indicate that the light adsorption capacity, carrier separation and transport efficiency of the optimized Co-BOC/BiOI-3 are greatly improved. This system demonstrates almost 100% removal rate for three typical EDCs within 60 min. The degradation kinetic constants show an improvement by an order of magnitude compared to single BiOI and Bi 2 O 2 CO 3 . More importantly, O 2 •﹣ , which is produced from O 2 reduction on high negative conduction band, can be subsequently oxidized into 1 O 2 by photogenerated hole. Electron paramagnetic resonance and quenching experiments indicate that the organics degradation process is dominated by 1 O 2 . This work offers new insights into the construction of high-quality S-scheme heterojunction interfaces for modulation of reactive oxygen species.
研究领域:
环境科学
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材料科学
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生物学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）