FUEL
·
2024
·
IF 6.7
Weijie Zhang,Lufang Fan,Kai Wei,Changchang Ma,Sheng Feng
This work provided innovative apertures with great exploratory value for engineering oxygen defects and designing S-scheme photocatalysts for efficient photocatalytic hydrogen production. In this study, the S-scheme heterostructure CdLa 2 S 4 /MoO 3-x (CLSMO) was synthesized by electrostatic self-assembly to solve the problem of electron hole recombination in hydrogen evolution half-reaction. The results showed that the hydrogen precipitation rate of the optimized CLSMO was 41.41 mmol g -1 h −1 , which was 12.70 times higher than that of monomeric CLS. The presence of oxygen vacancies (Ovs) increased the range of light absorption and reduces the surface dynamic barrier. More importantly, the experimental results and density functional theory (DFT) calculations showed that CdLa 2 S 4 and MoO 3-x strictly followed the S-scheme charge transfer path, accumulating photogenerated electrons in the CLS conduction band, and achieving efficient photocatalytic hydrogen evolution. This study provided a new idea to solve the problem of photocatalyst activity using OVs and S-scheme heterojunctions.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xinyi Chi,Mingyu Dou,Guang Yang,Ruixin Yang,Zunhao Wang,Hengyi Wang,Hua Yang,Wenning Yang,Erkang Liu,Jianmin Dou
The development of efficient and durable non-noble metal photocatalysts remains a major challenge, primarily owing to the fast recombination of photogenerated charge carriers and sluggish interfacial reaction kinetics. In this work, a ternary composite photocatalytic system, CdLa 2 S 4 /Mn 0.5 Cd 0.5 S-Co x P (CdLa 2 S 4 /MCS-Co x P), was rationally designed and constructed by coupling the S-scheme heterojunction with the metal-semiconductor Schottky interface, aiming to synergistically enhance multi-channel charge separation and migration. The construction of an S-scheme heterojunction comprising CdLa 2 S 4 and Mn 0.5 Cd 0.5 S (MCS) significantly facilitates the spatial separation of photogenerated electrons and holes driven by the built-in electric field, while simultaneously preserving their strong redox capability. Meanwhile, the Co x P acts as both an efficient electron acceptor and proton reduction site, its Schottky barrier at the interface further lowers the energy barrier for the hydrogen evolution reaction and accelerates surface reaction kinetics. Consequently, the CdLa 2 S 4 /MCS-Co x P composite exhibits a remarkable hydrogen evolution rate of 11.04 mmol g −1 h −1 , outperforming pristine MCS and CdLa 2 S 4 by factors of 10.32 and 38.07, respectively. This study offers a practical strategy for the rational design of multi-interface photocatalytic architectures with robust redox ability.
研究领域:
材料科学
·
催化
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纳米技术
·
能量转换
·
半导体物理
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Houfeng Zhang,Bojing Sun,Junjie Wang,Qian Zhu,Dongfang Hou,Chen Li,Xiu-qing Qiao,Dong-sheng Li
Optimize the separation and transport mechanism of photogenerated carriers in heterojunction composites, and make full use of the active sites of each material are key factors to enhance photocatalytic activity. Herein, we successfully synthesize defective CdLa 2 S 4 @La(OH) 3 @Co 3 S 4 (CLS@LOH@CS) Z-scheme heterojunction photocatalysts through a facile solvothermal method, which show broad-spectrum absorption and excellent photocatalytic activity. La(OH) 3 nanosheets not only greatly increase the specific surface area of photocatalyst, but also can be coupled with CdLa 2 S 4 (CLS) and form Z-scheme heterojunction by converting irradiation light. In addition, Co 3 S 4 with photothermal properties is obtained by in-situ sulfurization method, which can release heat to improve the mobility of photogenerated carriers, and also be used as a cocatalyst for hydrogen production. Most importantly, the formation of Co 3 S 4 leads to a large number of sulfur vacancy defects in CLS, and thus improving the separation efficiency of photogenerated electrons and holes, and increasing the catalytic active sites. Consequently, the maximum hydrogen production rate of CLS@LOH@CS heterojunctions can reach 26.4 mmol g -1 h −1 , which is 293 times than pristine CLS (0.09 mmol g -1 h −1 ). This work will provide a new horizon for synthesizing high efficiency heterojunction photocatalysts through switching the separation and transport modes of photogenerated carrier.
研究领域:
材料科学
·
化学
·
光催化
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Sujuan Zhang,Weixin Huang,Xianliang Fu,Xiuzhen Zheng,Sugang Meng,Xiangju Ye,Shifu Chen
Photocatalytic selective organic transformations (SOTs) with sunlight offer a “green” route for synthesis of fine chemicals. In this work, a bare ternary chalcogenide CdLa 2 S 4 photocatalyst was fabricated to couple the selective oxidation (SO) of aromatic alcohols to aldehydes and selective reduction (SR) of nitroarenes to anilines in one reaction system. The photocatalyst showed a high stability and a good generality for the conversions due to the well–matched band structure and the high separation efficiency of photoinduced electrons (e–) and holes (h + ). For p–substituted aromatic alcohols, the selectivities to the corresponding aldehydes are as high as ca. 90%. The electro–donating substituent in the para position benefits the SO reactions, which are triggered by h + via a successive deprotonation; while for p–substituted nitroarenes, the SR to the corresponding anilines is vulnerable to the electro–withdrawing groups and the steric hindrance of the substituent and the selectivities to anilines are substantially lower than that of the SO conversions. H + deprotonated in the SO of aromatic alcohols is indispensable for the SR of nitroarenes as they are achieved by a H + –coupled six e– reduction process, which leads to the low conversion efficiencies. The half conversions not only be coupled by the photoinduced e– and h + , but also collaborate with each other through H + . Our results clearly demonstrate the emerging concept of a coupled reaction system for sunlight–driven synthesis of fine chemicals and reveal the underlying mechanism.
研究领域:
光催化化学
·
有机合成
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材料化学
·
绿色化学
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物理化学
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半导体光催化
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精细化学品合成
✓ 已验证
DOI
高影响因子
RSC Advances
·
2012
·Vol. 2
·期 27
·10330-10336
·
IF 0
Jungang Hou,Chao Yang,Zheng Wang,Shuqiang Jiao,Hongmin Zhu
Large-scale hydrogen production through water splitting using photocatalysts with solar energy can potentially produce clean fuel from renewable resources. In this work, photocatalytic hydrogen evolution with a high efficiency was achieved using CdS nanocrystal decorated CdLa2S4 microspheres (CdS/CdLa2S4) successfully prepared by a two-step hydrothermal process. The obtained CdS/CdLa2S4 composite was characterized by X-ray diffraction (XRD), electron microscopy (EM), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance absorption spectroscopy (DRS), and photoluminescence spectroscopy (PL). XRD demonstrated that highly crystalline hexagonal CdS was obtained in CdS/CdLa2S4. EM results revealed that CdLa2S4 microspheres assembled from a large number of nanoprisms, were intimately enwrapped by the surrounding CdS nanocrystals with a particle size below 20 nm. This unique architecture resulted in the appropriate dispersion of CdS nanocrystals and intimate multipoint contacts between the CdS nanocrystals and CdLa2S4, which led to significant enhancement of charge separation in CdS/CdLa2S4. Especially, the CdLa2S4 microspheres decorated with 3 wt% CdS nanocrystals containing 0.4 wt% of Pt showed a high rate of H2-production at 2.25 mmol h−1 with an apparent quantum efficiency of 54% under 420 nm monochromatic light. The rate of hydrogen evolution from water splitting was 9 times faster in comparison with the rate observed on pure CdLa2S4, which is ascribed to the presence of CdS nanocrystals that alter the energy levels of the conduction and valence bands in the coupled semiconductor system.
研究领域:
材料科学
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光催化
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能源化学
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纳米材料
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半导体物理
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可再生能源
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催化化学
✓ 已验证
DOI
危险品化学品经营许可证（带存储）