CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zeshuang Kong,Jixian Dong,Jiahui Yu,Dafeng Zhang,Junchang Liu,Xue-Yang Ji,Peiqing Cai,Xipeng Pu
The construction of heterojunctions effectively suppresses the undesired recombination of photogenerated charge carriers. This work presents the rational design and preparation of a novel Cd 0.9 Zn 0.1 S/CoB (CZS/CoB) Schottky heterojunction tailored for photothermal-assisted photocatalytic hydrogen evolution with the aid of the predictions of density functional theory (DFT). Under visible light irradiation, the hydrogen evolution rate of CZS/CoB reaches 2.56 times that of pure CZS, due to the formed Schottky heterojunction and photothermal properties, effectively inhibiting electron-hole recombination and boosting the photocatalytic reaction. Notably, with the help of the excellent magnetic properties of CoB, the as-synthesized CZS/CoB exhibits excellent magnetic separation property, which is crucial for practical application. The charge transfer pathways in the Schottky heterojunction were confirmed by experimental results and verified by DFT calculation results. This study presents a feasible strategy for the design and preparation of magnetic recyclable Schottky Heterojunction photocatalyst for photocatalytic hydrogen evolution.
研究领域:
材料科学
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能源化学
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催化科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Zeshuang Kong,Jixian Dong,Jiahui Yu,Jinghao Cao,Xin liu,Dafeng Zhang,Junchang Liu,Peiqing Cai,Xipeng Pu
Easily recyclable photocatalysts hold great potential in the field of photocatalysis. Guided by rational theoretical predictions, this study designs a novel tetrapod-like Cd 0.9 Zn 0.1 S/NiCoB (CZS/NCB) Schottky heterojunction with magnetic and photothermal properties, and demonstrates its excellent photocatalytic hydrogen evolution performance. Under the combined effects of the photothermal properties and the Schottky heterojunction, the photocatalytic hydrogen evolution rate extraordinarily reaches 108.39 mmol g −1 h −1 after 3 h of visible light irradiation, which is 4.69 times that of pure CZS. Additionally, photocatalytic hydrogen evolution tests conducted using infrared thermography and alternating visible and visible plus infrared light irradiation have confirmed the material’s outstanding photothermal properties. In-depth density functional theory (DFT) calculations reveal potential charge transfer pathways and confirm the formation of the Schottky heterojunction. This work provides guidance for the rational construction of magnetic recoverable photocatalysts with practical application.
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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DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Dong Zhang,Minghui Zhu,Ran Qin,Peixian Chen,Maoye Yin,Dafeng Zhang,Junchang Liu,Hengshuai Li,Xipeng Pu,Peiqing Cai
Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology. In this study, the CuFe 2 O 4 @C/Cd 0.9 Zn 0.1 S (CFO@C/CZS) S-scheme photocatalyst with photothermal effect was synthesized by ultrasonic self-assembly combined with calcination. The dark CFO@C absorbed visible light and partly converted into heat to promote the hydrogen evolution reaction. The presence of heterojunctions inhibited the photogenerated electron-hole recombination. The graphite-carbon layer provided a stable channel for electron transfer, and the presence of magnetic CFO made recycle easier. Under the action of photothermal assistance and heterojunction, the hydrogen evolution rate of the optimal CFO@C/CZS was 80.79 mmol g −1 h −1 , which was 2.55 times and 260.61 times of that of pure CZS and CFO@C, respectively. Notably, the composite samples also exhibit excellent stability and a wide range of environmental adaptability. Through experimental tests and first-principles simulation calculation methods, the plausible mechanism of photoactivity enhancement was proposed. This work provided a feasible strategy of photothermal assistance for the development of heterojunction photocatalysts with distinctive hydrogen evolution.
研究领域:
材料科学
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环境科学
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能源科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Dong Zhang,Dafeng Zhang,Dong Fan,Junchang Liu,Hengshuai Li,Xipeng Pu,Haiquan Hu,Feng Guo,Peiqing Cai
Photocatalytic hydrogen production technology has emerged as one of the most promising technologies to address the future energy crisis. Cd0.9Zn0.1S (CZS) is a promising photocatalyst for visible light activation but is limited by the slow kinetics of photoexcited carrier separation. Density functional theory (DFT) calculations based on first-principles showed that the introduction of a cocatalyst, N-doped graphite carbon (FC@NC), could effectively reduce the adsorption free energy of hydrogen, thus accelerating the hydrogen reaction kinetics of CZS. Supported by theoretical predictions, magnetic FC@NC nanoparticles were successfully prepared by precipitation and calcination and then combined with tetrapod CZS by ultrasonic self-assembly and calcination to form the FC@NC/CZS composite photocatalyst with Schottky contact. The FC@NC/CZS composite photocatalyst with the best mass ratio of FC@NC proved a considerable photocatalytic hydrogen evolution rate up to 79.9 ± 0.1 mmol g–1 h–1 under visible light exposure, which was 4.4 ± 0.1 times that of pristine CZS, and the apparent quantum efficiency (AQE) at 450 nm was as high as 52%. Finally, based on the experimental results and DFT calculations, a possible mechanism for the enhanced photocatalytic activity of FC@NC/CZS composites with the Schottky heterojunction was first proposed. In general, we attribute the boosted and stable photocatalytic property of FC@NC/CZS photocatalytic performance to the following three aspects: (1) the bimetallic alloy cocatalyst easily acts as an electron collector, (2) the graphite carbon layer protects the alloy from oxidation, and (3) the nitrogen-doped carbon layer provides more active sites for the reaction. This work provided a green and economical technique for an efficient hydrogen evolution reaction using light energy in the environment.
研究领域:
材料科学
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能源科学
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Zeshuang Kong,Dong Zhang,Jixian Dong,Jiahui Yu,Dafeng Zhang,Junchang Liu,Peiqing Cai,Xipeng Pu
Within the theoretical framework of computational prediction, this study introduces a novel tetrapodal Cd 0.9 Zn 0.1 S/NiB (CZS/NiB) Schottky heterojunction material, which demonstrates exceptional photothermal effects and remarkable photocatalytic properties. Notably, under visible light irradiation for 3 h, the photocatalytic hydrogen evolution activity of CZS/NiB-3 % surpasses that of pure CZS by a factor of 10.52. This outstanding photocatalytic hydrogen production performance stems from the successful construction of the CZS/NiB-3 % Schottky heterojunction with promoted the separation and transfer of photogenerated charge carriers and excellent photothermal effect. Additionally, the synthesized CZS/NiB exhibits high photostability and cycling stability. The favorable photothermal effect of the synthesized photocatalyst was experimentally validated through infrared thermography technology. Through in-depth computational investigations using density functional theory, the pathways of charge transfer in the Schottky heterojunction are validated. This study provides a feasible strategy for research on photocatalytic water splitting for hydrogen evolution.
研究领域:
材料科学
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能源化学
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计算化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2020
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IF 6.146
Zhuwang Shao,Xiao Meng,Hong Lai,Dafeng Zhang,Xipeng Pu,Changhua Su,Hong Li,Xiaozhen Ren,Yanling Geng
In this study, Ni 2 P-Cd 0.9 Zn 0.1 S (NPCZS) composites were synthesized by coupling tetrapod bundle Cd 0.9 Zn 0.1 S (CZS) and coralline-like Ni 2 P (NP) via a simple calcination method. CZS shows outstanding activity in photocatalytic hydrogen evolution (1.31 mmol h −1 ), owing to its unique morphology and heterophase homojunctions (ZB/WZ), which accelerate the separation and transfer of photogenerated charges. After coupling with NP, the photoactivity of NPCZS was enhanced, and the maximum hydrogen evolution rate of 1.88 mmol h −1 was reached at a NP content of 12 wt%, which was 1.43 times higher than that of pure CZS. The experimental results of the photocatalytic activity, viz. photoluminescence spectra, surface photovoltage spectra, and electrochemical test showed that the enhanced photoactivity of NPCZS should be attributed to the synergistic effects of the novel tetrapod-bundle morphology, heterophase homojunctions, and decoration of the NP co-catalyst. Moreover, the as-prepared NPCZS composites exhibited excellent photostability and recyclability. Herein, we propose a possible mechanism for the enhanced photocatalytic activity.
研究领域:
材料科学
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能源化学
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光催化技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Meixuan Cai,Ruobai Li,Zhijie Xie,Jiaxing Huang,Yongqin Zeng,Qianxin Zhang,Haijin Liu,Wenying Lv,Guoguang Liu
The development of novel noble metal-free semiconductor catalysts with high photocatalytic efficiency is of great importance toward the degradation of organic compounds. In this work, a core-shell heterojunction MoS 2 /Cd 0.9 Zn 0.1 S photocatalytic material was successfully synthesized via a simple one-step hydrothermal method. The introduction of MoS 2 led to a significant improvement in the photocatalytic degradation of diclofenac (DCF). It was confirmed that 0.1% loading content of MoS 2 achieved an optimal photocatalytic efficiency of 86% in the degradation of DCF under visible light irradiation, which was 1.8 times higher than that of Cd 0.9 Zn 0.1 S. The MoS 2 /Cd 0.9 Zn 0.1 S heterostructured composites possessed improved photocatalytic properties, which implied that the combination of Cd 0.9 Zn 0.1 S and MoS 2 shortened the carrier transport pathway and facilitated the separation efficiency of electrons and holes. Reactive species (RS) scavenging experiments and electron spin resonance (ESR) demonstrated that superoxide radicals (O 2 •− ) and electron holes (h + ) played predominant roles throughout the DCF degradation process. The primary intermediates were explored through HRAM LC/MS/MS, and a transformation pathway was tentatively proposed. This study promoted the application of an economical, highly efficient and visible light driven MoS 2 co-catalyst for the degradation of organic contaminants.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ping Su,Shikai Wang,Dong Zhang,Tengteng Liang,Huaihao Zhao,Nan Yang,Dafeng Zhang,Peiqing Cai,Xipeng Pu
Rational design of photocatalysts with photothermal effect to maximize light utilization is pivotal in achieving superior photocatalytic efficiency. In this work, by coating Cd 0.9 Zn 0.1 S (CZS) nanorods on hollow FeNi 2 S 4 (FNS) microspheres with photothermal effect, a novel FeNi 2 S 4 @Cd 0.9 Zn 0.1 S (FNS@CZS) Step-scheme (S-scheme) heterojunction photocatalyst was constructed for efficient photothermal-assisted hydrogen (H 2 ) evolution via simultaneously employing light and thermal energy. The hollow structure of FNS microsphere not only provides abundant reactive sites but also serves as a supportive substrate for CZS nanorods, effectively inhibiting their agglomeration. And the unique hollow structure of FNS allows for multiple reflections and refractions of visible light, enhancing the local temperature of the photocatalyst. This effectively minimizes thermal losses within the composite system, thereby enhancing the efficiency of light energy utilization. Furthermore, the formation of the S-scheme heterojunction facilitates the efficient separation of photogenerated charge carriers and enhances the activity of redox reactions, thereby boosting the overall photocatalytic activity. Experimental results reveal that the H 2 production rate of the FNS@CZS heterojunction reaches 12.9 mmol·g −1 ·h −1 , which is 25.1 times higher than that of pristine CZS. By controlling the experimental temperature, the impact of the photothermal effect on the photocatalytic H 2 production rate has been clarified. According to relevant evidence from infrared thermography and DFT calculations, comprehensive analyses and discussions were conducted on the photothermal effect and S-scheme charge transfer mechanisms. This study offers guidance on designing photothermal-enhanced photocatalysts to achieve satisfactory H 2 production activity.
研究领域:
材料科学
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能源化学
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环境科学
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DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Ping Su,Dong Zhang,Minghui Zhu,Tengteng Liang,Nan Yang,Huaihao Zhao,Dafeng Zhang,Junchang Liu,Peiqing Cai,Xipeng Pu
Piezoelectric materials have advantages of fine-tuning photocatalytic performance through harvesting mechanical energy and open a new avenue in facilitating green catalytic reaction. Herein, polyvinylidene fluoride (PVDF), a flexible piezoelectric material, was introduced to synthesize a novel Cd 0.9 Zn 0.1 S-ZnO@C/PVDF (CZS-ZO@C/PVDF) piezo-photocatalytic film by spin coating and immersion phase conversion method. Benefiting from the piezoelectricity of PVDF and the internal electric field (IEF) of CZS-ZO@C Step-scheme (S-Scheme) heterojunction, CZS-ZO@C/PVDF was able to induce a hydrogen generation rate of 34.9 mmol g −1 h −1 activated by ultrasound and visible light (U-L), which is ∼17.5 times of Cd 0.9 Zn 0.1 S/PVDF (CZS/PVDF) and ∼7.4 times of the photocatalysis rate activated by visible light only (L). Piezoelectric measurements and COMSOL simulation illustrated the excellent piezoelectricity of CZS-ZO@C/PVDF film, which exhibits a piezoelectric coefficient ( d 33 ) of 9.9 pm V −1 and a piezoelectric potential of 874 mV (under 0.5 MPa). The reaction mechanism for the exceptional piezo-photocatalytic performance was finally disclosed through density functional theory (DFT) calculation and electrochemical tests. This study enriches the application scope of piezoelectric materials in sustainable energy catalysis and provides a new direction to develop efficient piezoelectric photocatalysts.
研究领域:
材料科学
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催化
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可再生能源
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纳米技术
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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
Dafeng Zhang,Dong Zhang,Shikai Wang,Hengshuai Li,Junchang Liu,Xipeng Pu,Peixian Chen,Ran Qin,Haiquan Hu,Peiqing Cai
Suppressing the electron-hole recombination rate of catalyst legitimately is one of the effective strategies to improve photocatalytic hydrogen evolution . Herein, carbon-coated metal oxide , ZnFe 2 O 4 @C (ZFO@C), nanoparticles were synthesized and employed to couple with quadrupedal Cd 0.9 Zn 0.1 S (CZS) via an ordinary ultrasonic self-assembly method combined with calcination to form a novel ZFO@C/CZS catalyst with step-scheme (S-scheme) heterojunction . The photocatalytic hydrogen evolution reaction (HER) was conducted to verify the enhanced photoactivity of ZFO@C/CZS. The optimal ZFO@C/CZS exhibits an extraordinary photocatalytic HER rate of 111.3 ± 0.9 mmol g -1 h −1 under visible-light irradiation, corresponding to an apparent quantum efficiency as high as (76.2 ± 0.9)% at 450 nm. Additionally, the as-synthesized ZFO@C/CZS composite exhibits high stability and recyclability. The excellent photocatalytic hydrogen evolution performance should arise from the formed S-scheme heterojunction and the unique ZFO@C core–shell structure, which inhibit electron hole recombination as well as provide more reactive sites. The pathway of S-scheme charge transfer was validated through density functional theory calculations and electrochemical measurements. This work provides a rational strategy for the synthesis of unique magnetic S-scheme heterojunction photocatalysts for water splitting under visible light irradiation.
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Caicai Ran,Mang Lu,Linli Hou,Huanggen Yang,Limin Liu
Heterogeneous interface regulation acts a significant role in tailoring the intrinsic physicochemical property for achieving excellent photocatalytic H 2 evolution performance, which still faces a huge challenge. In this work, by comparing H 2 evolution property of various cadmium zinc sulphide (Cd x Zn 1−x S) solid solutions, 1-D Cd 0.9 Zn0 .1 S nanorods possessing the optimum photocatalytic H 2 evolution performance were obtained. Additionally, bimetallic metal organic framework (MOF)-derived NiFe 2 O 4 @C (NFO@C) microspheres with custom-built heterogeneous interface were successfully prepared via a solvothermal/pyrolysis strategy. Moreover, NFO@C microspheres were assembled on Cd 0.9 Zn0 .1 S surface to fabricate a series of NFO@C/Cd 0.9 Zn 0.1 S heterojunction photocatalysts with varied contents of NFO@C. The NFO@C/Cd 0.9 Zn 0.1 S heterojunction with a NFO@C content of 20 wt% (abbreviated as NC20) exhibited the highest H 2 production rate of 96.25 mmol g –1 h −1 , which was 3.8 times that of Cd 0.9 Zn 0.1 S. Under a light wavelength of 420 and 450 nm, the apparent quantum efficiency of NC20 reached 34.8 % and 65.1 %, respectively. The photocatalytic H 2 evolution activity of NC20 remained stable after the 16-h cycle experiment, whereas the severe photocorrosion of Cd 0.9 Zn 0.1 S was encountered. Furthermore, the easy recyclability of NC20 should not be overlooked. The results of a series of material characterization clearly demonstrate that the introduction of NFO@C could efficiently improve light absorption and the photoinduced carrier separation capability of the composite photocatalysts. This study not only opens up a facile and controllable preparation way for the synthesis of heterojunction structures with tailored heterogeneous interfaces, but also offers a new sight to ameliorate the H 2 evolution capability, stability and recyclability of Cd x Zn 1−x S solid solutions.
研究领域:
材料科学
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光催化
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氢能
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纳米材料
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异质结工程
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DOI
高影响因子
CERAMICS INTERNATIONAL
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2026
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IF 6
Chengkai Li,Changjian Zhou,Ze Liu,Zhenyu Zhang,Danni Zeng,Rongfeng Guan
Driven by the dual demands of global energy structure transformation and carbon neutrality goals, solar-driven green hydrogen and green chemical synthesis have become a focus. This study employs a Prussian blue template to guide the one-step synthesis of Cu/Ni co-doped Cd 0.9 Zn 0.1 S, which not only retains a high-surface-area porous framework with exposed active sites but also intentionally introduces abundant sulfur vacancies (Vs). The synergistic interplay of Cu doping (acting as electron-rich centers), Ni doping (serving as hole-trapping centers), and the generated V s collectively optimizes the band structure, extends light absorption to nearly 700 nm, and significantly enhances charge carrier separation. The optimized 10Cu/10Ni- Cd 0.9 Zn 0.1 S photocatalyst achieves an exceptional hydrogen production rate of 21.25 mmol g −1 h −1 (20-fold enhancement) and a H 2 O 2 production rate of 4.6 mmol g −1 h −1 under oxygen conditions (15-fold enhancement). Remarkably, the in-situ generated H 2 O 2 is efficiently activated on Cu/Ni sites and Vs via a photo-Fenton-like process, enabling rapid tetracycline degradation (94% within 40 min). DFT calculations reveal that the hydrogen adsorption free energy is optimized to −0.09 eV, and the introduced sulfur vacancies further lower the work function, promoting O 2 activation and charge transfer for both H 2 evolution and Fenton-like reactions. This study offers new insights into designing highly efficient photocatalysts by employing a coupled doping and vacancy engineering strategy to synergistically regulate redox-active sites, combining porous framework design for optimized mass transport and multifunctional environmental remediation.
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DOI
高影响因子
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