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1.
In this work, the Mn0.2Cd0.8S/NiCo2O4 composite modified with Ni2P as a co-catalyst was fabricated via a simple two-step hydrothermal method. The as-prepared ternary Mn0.2Cd0.8S/NiCo2O4/Ni2P composite displayed excellent H2 production performance. The ternary composite loaded with 5 wt% NiCo2O4 and 2 wt% Ni2P obtained the optimal H2 production performance of 24.47 mmol g?1 h?1 and a maximum AQE of 23.75%. The enhanced H2 production activity was assigned firstly to efficient spatial charge separation through the p?n Mn0.2Cd0.8S/NiCo2O4 heterojunction and secondly to sufficient surface active sites provided by Ni2P co-catalysts. This research provides a new approach to design effective ternary heterojunction.  相似文献   

2.
Photocatalytic hydrogen evolution from water splitting is a promising strategy to solve the energy demand of human beings. Here, we first designed a C–Mn0.5Cd0.5S/Cu3P ternary heterojunction catalyst for photocatalytic hydrogen production. The results show that the combination of C and Cu3P can effectively improve the photocatalytic activity of Mn0.5Cd0.5S. C–Mn0.5Cd0.5S loading with 5 wt% Cu3P exhibits the highest hydrogen evolution rate (44.1 mmol g−1 h−1), which is 3.2 and 2.8 times higher than that of pure Mn0.5Cd0.5S (13.7 mmol g−1 h−1) and Mn0.5Cd0.5S/3 wt%Pt (15.6 mmol g−1 h−1), respectively. In addition, it shows a high hydrogen evolution rate (19.6 mmol g−1 h−1) under visible light (≥420 nm) irritation and the apparent quantum efficiency (AQE) is detected to be 3.2% at 420 nm. The enhanced photocatalytic activity can be attributed to the good conductivity of C and the formation of p-n heterojunction, which is beneficial for light harvesting and the separation and transportation of charge carriers. Besides, a possible mechanism is proposed. This work provides an effective way to improve the photocatalytic activity of Mn0.5Cd0.5S by using non noble metal co-catalysts.  相似文献   

3.
Designing an efficient non-noble metal photocatalyst, which utilizes solar energy, has great potential to produce clean energy hydrogen. The microstructural refinement of 1D Cd0.2Zn0.8S nanorod was induced by doping with 2D MoS2@MoOy layer during microwave hydrothermal treatment. The maximum H2 production rate of the composite prepared at optimum conditions was 186 mmol g−1 h−1, which increased by 34.8% compared with that of Cd0.2Zn0.8S (138 mmol g−1 h−1). The apparent quantum yields of the optimized composite were 10.3% and 15.6% at 365 and 420 nm, respectively. The tight S-scheme heterojunction contributed to the separation of photogenerated electron-hole pairs effectively, as confirmed by the characterization analysis of ·OH and ·O2 radicals, surface potential under illumination and darkness and in situ XPS spectra. Moreover, the active species of sulfur coordinated-Mo5+ as low-coordinate center promoted the dissociation of water and decreased the over potential of H2 production. Furthermore, the optimal composite showed excellent stable catalytic activity for hydrogen evolution, and the H2 production rate was 176.7 mmol g−1 h−1 after five cycles (95% of the first cycle). Overall, this work provides a promising strategy for improving the effectiveness of H2 production by preparing non-noble metal composite photocatalysts.  相似文献   

4.
In this work, Mo3S4/Cd0.5Zn0.5S heterojunction with abundant porosity was in-situ synthesized by one-step hydrothermal method. Characterization results clearly indicate that the composite material are composed of nanoparticles with an average particle diameter about 65 nm and abundant inter-particle pores are present in between. The XPS analysis found that when Mo3S4 was introduced, the XPS peak positions of Cd2+ and Zn2+ were shifted from the XPS peak positions of Cd2+ and Zn2+ in pristine Cd0.5Zn0.5S, which indicates that there is an interaction between Mo3S4 and Cd0.5Zn0.5S at the interface. Subsequently, the Mo3S4/Cd0.5Zn0.5S (72.1 mmol h−1 g−1) heterojunction can achieve much higher photocatalytic hydrogen production rate than the pristine Cd0.5Zn0.5S (7.54 mmol h−1 g−1), and even higher than Cd0.5Zn0.5S (56.44 mmol h−1 g−1) loaded with the noble metal Pt (2.0%), indicating that heterojunction can effectively enhance photocatalytic activity. In addition, the improvement in photocatalytic activity of Mo3S4/Cd0.5Zn0.5S is highly related with enhanced absorption and utilization of light due to the presence of the inter-particle pores which inhibit recombination of electron-hole pairs, promote charge separation and accelerate the migration of photogenerated carriers.  相似文献   

5.
The development of photocatalysts with efficient hydrogen evolution activity has been the goal for sustainable hydrogen production. In this work, heterojunction composite photocatalyst is formed by hydrothermal coupling of ZnO and Mn0.2Cd0.8S. Compared with pure ZnO and Mn0.2Cd0.8S, the composite photocatalyst has the ability to provide more abundant active sites and better photogenerated carriers separation efficiency. The optimized composite photocatalyst shows a 9.36-fold increase in hydrogen evolution activity (4297.99 μmol g?1 h?1) compared to Mn0.2Cd0.8S (459.31 μmol g?1 h?1) and exhibits excellent cycling stability. Density functional theory calculations identifies Type-II charge transfer path in the composite photocatalyst, achieving effective separation in space of photogenerated electrons from holes and suppressing recombination within the semiconductor. The results show that the construction of Type-II heterojunction in this work achieves a significant enhancement of the hydrogen evolution activity of the photocatalyst by constructing carrier transport channels at the contact interface of the heterojunction.  相似文献   

6.
The design of p-n heterojunction photocatalysts to overcome the drawbacks of low photocatalytic activity that results from the recombination of charge carriers and narrow photo-response range is promising technique for future energy. Here, we demonstrate the facile hydrothermal synthesis for the preparation of Bi2O3/MoS2 p-n heterojunction photocatalysts with tunable loading amount of Bi2O3 (0–15 wt%). The structure, surface morphology, composition and optical properties of heterostructures were studied using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), UV–visible absorption spectroscopy, Brunauer-Emmett-Teller (BET) surface area, photoluminescence (PL), electrochemical impedance spectroscopy (EIS). Compare to pure Bi2O3 and MoS2, the Bi2O3/MoS2 heterostructures displayed significantly superior performance for photocatalytic hydrogen (H2) production using visible photo-irradiation. The maximum performance for hydrogen evolution was achieved over Bi2O3/MoS2 photocatalyst (10 μmol h−1g−1) with Bi2O3 content of 11 wt%, which was approximately ten times higher than pure Bi2O3 (1.1 μmol h−1g−1) and MoS2 (1.2 μmol h−1g−1) photocatalyst. The superior performance was attributed to the robust light harvesting ability, enhanced charge carrier separation via gradual charge transferred pathway. Moreover, the increased efficiency of Bi2O3/MoS2 heterostructure photocatalyst is discussed through proposed mechanism based on observed performance, band gap and band position calculations, PL and EIS data.  相似文献   

7.
In recent years, tremendous efforts have been devoted to develop new photocatalyst with wide spectrum response for H2 generation from water or aqueous solution. In this paper, MnxCd1-xS composites were in-situ fabricated via the high-temperature sulfurization to enhance the solar-light photocatalytic capacity of H2 evolution. Benefiting from the S defects and junction interface between MnS and CdS, MnxCd1-xS composites exhibited the better H2 evolution rate than pure MnS. The H2 evolution rate of optimal Mn0.5Cd0.5S with a Mn(II) content of 22.52% and a Mn/Cd mole ratio of 0.95:1 was 9.27 mmol g?1 h?1, which was 35.65 and 2.38 times higher than pure MnS (0.26 mmol g?1 h?1) and CdS (3.89 mmol g?1 h?1), respectively. In addition, H2 evolution capacity of Mn0.5Cd0.5S decreased from 44.83 to 41.66 mmol g?1 after three cycles. Mn0.5Cd0.5S prepared via the high-temperature sulfurization was thus a potential material for solar-light induced H2 generation.  相似文献   

8.
Excellent light harvest, efficient charge separation and sufficiently exposed surface active sites are crucial for a given photocatalyst to obtain excellent photocatalytic performances. The construction of two-dimensional/two-dimensional (2D/2D) or zero-dimensional/2D (0D/2D) binary heterojunctions is one of the effective ways to address these crucial issues. Herein, a ternary CdSe/WS2/g-C3N4 composite photocatalyst through decorating WS2/g-C3N4 2D/2D nanosheets (NSs) with CdSe quantum dots (QDs) was developed to further increase the light harvest and accelerate the separation and migration of photogenerated electron-hole pairs and thus enhance the solar to hydrogen conversion efficiency. As expected, a remarkably enhanced photocatalytic hydrogen evolution rate of 1.29 mmol g−1 h−1 was obtained for such a specially designed CdSe/WS2/g-C3N4 composite photocatalyst, which was about 3.0, 1.7 and 1.3 times greater than those of the pristine g-C3N4 NSs (0.43 mmol g−1 h−1), WS2/g-C3N4 2D/2D NSs (0.74 mmol g−1 h−1) and CdSe/g-C3N4 0D/2D composites (0.96 mmol g−1 h−1), respectively. The superior photocatalytic performance of the prepared ternary CdSe/WS2/g-C3N4 composite could be mainly attributed to the effective charge separation and migration as well as the suppressed photogenerated charge recombination induced by the constructed type-II/type-II heterojunction at the interfaces between g-C3N4 NSs, CdSe QDs and WS2 NSs. Thus, the developed 0D/2D/2D ternary type-II/type-II heterojunction in this work opens up a new insight in designing novel heterogeneous photocatalysts for highly efficient photocatalytic hydrogen evolution.  相似文献   

9.
Designing cost-effective photocatalysts with remarkable performance is a foresighted strategy to foster the evolution of H2 in water splitting. In this study, a p-n heterojunction FeWO4/Mn0.5Cd0.5S photocatalyst modified by low-cost and non-toxic FeWO4 was synthesized using hydrothermal and calcination methods. The hydrogen evolution activity of Mn0.5Cd0.5S was strengthened by varying the amount of FeWO4 loading. The hydrogen production rate of FeWO4/Mn0.5Cd0.5S photocatalyst loaded with 10% FeWO4 can reach 9.63 mmol g?1 h?1, which is equivalent to 2.16 times of pure Mn0.5Cd0.5S. The enhancement of the H2 evolution activity was primarily contributed to a p-n heterojunction formed at the interface of FeWO4 and Mn0.5Cd0.5S. It provides a fast pathway for the migration and separation of photogenerated charges and effectively inhibits the photo-corrosion of Mn0.5Cd0.5S.  相似文献   

10.
An oxygen-vacancy rich, bismuth oxide (Bi2O3) based MoS2/Bi2O3 Z-scheme heterojunction catalyst (2-BO-MS) was prepared in an autoclave hydrothermal method using ethanol and water. The performance of MoS2/Bi2O3 catalyst was examined for photocatalytic hydrogen evolution, photoelectrochemical activity, and crystal violet (CV) dye degradation by comparing with pristine Bi2O3 and MoS2. The hydrogen evolution performances of 2-BO-MS catalyst exhibited 3075.21 μmol g−1 h−1, which is 7.18 times higher than that of MoS2 (428.14 μmol g−1 h−1). The XPS, XRD and HRTEM analyses covered that the superior photocatalytic performance of 2-BO-MS catalyst might have stemmed out due to the existence of oxygen vacancies, enhanced strong interfacial interaction between MoS2 and Bi2O3 and specific surface area. The in-depth investigation has been performed for MoS2/Bi2O3 Z-scheme heterojunction using several characterization techniques. Moreover, the photocatalytic mechanism for hydrogen evolution and photodegradation were proposed based on trapping experiment results. This results acquired using MoS2/Bi2O3 Z-scheme heterojunction would be stepping stone for developing heterojunction catalyst towards attaining outstanding photocatalytic activity.  相似文献   

11.
The Z-scheme heterojunction photocatalysts possess excellent photocatalytic activity benefitting from their properly matched edge potentials. In this work, ZnCo2S4 nanoparticles are anchored on Zn0.2Cd0.8S solid solution nanowires and assembled into binary ZnCo2S4/Zn0.2Cd0.8S nanocomposites. The as-synthesized ZnCo2S4/Zn0.2Cd0.8S nanocomposites act as bifunctional photocatalysts, which can be used for high-performance H2 production coupling synthesis of high-value-added benzaldehyde in low concentration benzyl alcohol solution. Under visible light irradiation, 20%-ZnCo2S4/Zn0.2Cd0.8S nanocomposite shows the highest H2 evolution rate of 23.02 mmol g?1 h?1 in the first photocatalytic cycle, which is 395.0 and 526.7 times higher than that of Zn0.2Cd0.8S and ZnCo2S4 under the same conditions. Eventually, after six-time cycles, the conversion rate and selectivity of benzyl alcohol oxidation to benzaldehyde are 54.3% and 92.2%, respectively. The enhancement of photocatalytic performance is mainly attributed to the Z-scheme heterojunction between ZnCo2S4 and Zn0.2Cd0.8S, which promote the separation and transfer of photogenerated charge carriers. This work provides strong support for the rational design of Z-scheme nano-heterojunction of highly efficient photocatalytic application in H2 evolution and fine chemicals production.  相似文献   

12.
Constructing heterostructures with efficient charge separation is a promising route to improve photocatalytic hydrogen production. In this paper, MoSx/CdS/KTaO3 ternary heterojunction photocatalysts were successfully prepared by a two-step method (hydrothermal method and photo deposition method), which improved the photocatalytic hydrogen evolution activity. The results show that the rate of hydrogen evolution for the optimized photocatalyst is 2.697 mmol g?1·h?1under visible light, which is 17 times and 2.6 times of the original CdS (0.159 mmol g?1 h?1) and the optimal CdS/KTaO3(1.033 mmol g?1 h?1), respectively, and the ternary photocatalyst also shows good stability. The improvement on photocatalytic hydrogen evolution performance can be attributed to the formation of heterojunction between the prepared composite materials, which effectively promotes the separation and migration of photo-generated carriers. Amorphous MoSx acts as an electron trap to capture photogenerated electrons, providing active sites for proton reduction. This provides beneficial enlightenment for hydrogen production by efficiently utilizing sunlight to decompose water.  相似文献   

13.
A binary heterostructured CdS/MoS2 flowerlike composite photocatalysts was synthesized via a simple one-pot hydrothermal method. This photocatalyst demonstrated higher photocatalytic hydrogen production activity than pure MoS2. The heterojunction formed between MoS2 and CdS seems to promote interfacial charge transfer (IFCT), suppress the recombination of photogenerated electron–hole pairs, and enhance the hydrogen generation. Based on the good match between the conduction band (CB) edge of CdS and that of MoS2, electrons in the CB of CdS can be transferred to MoS2 easily through the heterojunction between them, which prevents the accumulation of electrons in the CB of CdS, inhibiting photocorrosion itself and greatly enhancing stability of catalyst. Hydrogen evolution reaction (HER) using Na2S/Na2SO3 or glucose as sacrificial agents in aqueous solution was investigated. The ratio between CdS and MoS2 plays an important role in the photocatalytic hydrogen generation. When the ratio between CdS and MoS2 reaches 40 wt%, the photocatalyst showed a superior H2 evolution rate of 55.0 mmol g−1 h−1 with glucose as sacrificial agent under visible light, which is 1.2 times higher than using Na2S/Na2SO3 as sacrificial agent. Our experimental results demonstrate that MoS2-based binary heterostructured composites are promising for photocorrosion inhibition and highly efficient H2 generation.  相似文献   

14.
Designing efficient photocatalytic systems for hydrogen evolution is extremely important from the viewpoint of the energy crisis. Highly crystalline heterostructure catalysts have been established, considering their interface electric field effect and structural features, which can help improve their photocatalytic hydrogen-production activity. In this study, we fabricated a highly crystalline heterojunction consisting of ZnFe2O4 nanobricks anchored onto 2D molybdenum disulfide (MoS2) nanosheets (i.e., ZnFe2O4/MoS2) via a hydrothermal approach. The optimized ZnFe2O4/MoS2 photocatalyst, with a ZnFe2O4 content of 7.5 wt%, exhibited a high hydrogen-production rate of 142.1 μmol h−1 g−1, which was 10.3 times greater than that for the pristine ZnFe2O4 under identical conditions. The photoelectrochemical results revealed that the ZnFe2O4/MoS2 heterojunction considerably diminished the recombination of electrons and holes and promoted efficient charge transfer. Subsequently, the plausible Z-scheme mechanism for photocatalytic hydrogen production under white-LED light irradiation was discussed. Additionally, the influence of cocatalysts on the photocatalytic hydrogen evolution for the ZnFe2O4/MoS2 heterostructure was investigated. This work has demonstrated a simplified coupling of one-dimensional or zero-dimensional structures with 2D nanosheets for improving the photocatalytic hydrogen production activity as well as confirmed that MoS2 is a viable substitute for precious metal-free photocatalysis.  相似文献   

15.
Bimetallic compounds nanocrystals exhibited great potential in catalysis due to the synergistic effects and encouraging performance. Herein, a series of NiCo-based nanosheets, including NiCo LDH/NiCo(OH)2, NiCo, and NiCo2O4, have been developed to modify MnS/Mn0·2Cd0·8S (MMCS) nanoparticles for photocatalytic H2 production under visible light (λ > 420 nm). The two-dimensional (2D) NiCo2O4 and NiCo were derived from the oxidation and reduction process of the as-prepared NiCo LDH/NiCo(OH)2 nanosheets, respectively. MMCS nanoparticles were prepared using a one-pot solvothermal method and then integrated into three different NiCo-based nanosheets through a simple hybridization approach. Compared to pure MMCS, the resultant NiCo-based nanosheets/MMCS hybrids show dramatically improved visible-light photocatalytic activities. Moreover, among the three types of composites, NiCo2O4-MMCS (7%NiCo2O4-MMCS) displays the highest H2 production rate of 3.31 mmol g?1 h?1 with the apparent quantum efficiency of 6.42% at 420 nm, approximately 22 and 5 times that of pure MMCS (0.15 mmol g?1 h?1) and Pt/MMCS (0.67 mmol g?1 h?1), respectively. The remarkably enhanced photocatalytic activities of the NiCo LDH/NiCo(OH)2-MMCS, NiCo-MMCS, and NiCo2O4-MMCS are mainly ascribed to the formed type-II, Schottky, and p-n heterojunctions, respectively, which efficiently boost photogenerated charge carrier separation and migration. In this paper, we intensively investigate the roles of three different NiCo-based nanosheets in the MnxCd1-xS-based system. This work provides an effective strategy to design and construct the innovative 2D bimetallic compounds-based catalysts for high-efficiency photocatalytic H2 production.  相似文献   

16.
The study investigated the synergistic effects of rGO and Pt over TiO2 for the HER via artificial photosynthesis under UVB and visible light irradiation. The introduction of glycerol and industrial wastewater to the system as sacrificial reductants signifies that the major reaction pathway is photocatalytic partial water splitting. The material characterizations revealed successful heterojunction formation and provided insight into chemistry behind the activity of the photocatalysts. Amongst various combinations of rGO on TiO2, 1GNT exhibited an HER yield five times that of bare TiO2 under UVB light. Addition of Pt led to the formation of a strong Schottky barrier at the heterojunction and consequently boosted HER performance. 1P0.5 GT presented the highest of 28.5 mmol g−1 h−1 with glycerol and 9.6 mmol g−1 h−1 with wastewater under UVB light respectively. For both binary and ternary photocatalysts, the HER performances dwindled under visible light irradiation, accentuating the insufficient activation of the TiO2. In addition, 1PT outperformed all the other photocatalysts thereby elucidating the impression that rGO and Pt does not work well together in enhancing HER despite quenching the exciton recombination rate of TiO2 significantly. The role of pH in the synthesis and the experiments has been discussed. Finally, the underlying mechanisms in the photodeposition and photoreformation have been proposed.  相似文献   

17.
In this work, p-type semiconductor CoWO4 nanoparticles was successfully anchored on the surface of n-type Mn0.2Cd0.8S nanorods, and p-n type heterostructure photocatalysts with low cost and high efficiency were synthesized. By optimizing the loading of CoWO4 nanoparticles, the hydrogen evolution rate of the compound can reach a maximum, the peak is 408 μmol/5 h. Under visible light irradiation, it is equivalent to 3.61 times pure Mn0.2Cd0.8S. In addition, the composite catalyst has favorable durability and structural stability. In terms of morphology, the combination of nanorods (SBET = 24 m2g-1) and nanoparticles (SBET = 12 m2g-1) increased the specific surface area of the composite catalyst (SBET = 31 m2g-1), thus the composite exposed more active sites. In terms of heterojunction, the conduction bands of two semiconductors were determined by UV–vis diffuse reflection and Mott-Schottky, and the construction of p-n heterojunction was verified. The results of photochemical experiment further indicate that the built-in electric field in the p-n type heterostructure not only accelerates the electron-hole pair transfer, but vastly enhances the carrier average lifetime. In this paper, the morphology of the photocatalyst was modified and p-n heterojunction was constructed. The result is that the performance of Mn0.2Cd0.8S MCS was improved and the possible mechanism of photocatalytic hydrogen evolution was proposed.  相似文献   

18.
A designed type-II heterojunction photocatalyst, NiSe2/Cd0.5Zn0.5S (NiSe2/CZS), was successfully synthesized and it exhibits outstanding photocatalytic hydrogen evolution performance. The optimal loading amount of NiSe2 on Cd0.5Zn0.5S is 13 wt %, and the corresponding hydrogen production rate is approximately 121.01 mmol g?1 h?1 under visible light. The heterojunction structure between Cd0.5Zn0.5S and NiSe2 promoted the separation of photogenerated electron-hole pairs, effectively suppressed the photogenerated carrier recombination and endowed the material with excellent interfacial charge transfer properties, thus improving the photocatalytic performance.  相似文献   

19.
Solar-light driven water splitting acted as an important technology to solve the energy crisis has attracted much more attention. To restrain the recombination rate of charge carriers and enhance the surface activity of TiO2, integrating dual CdS–CoS with S,N-codoped TiO2 with a Cd/Co mole ratio of 1:1 (Cd0.5Co0.5S/SN-TiO2) nano-fibers were fabricated via the electro-spinning and one-pot hydrothermal routes. H2-evolution rate of Cd0.5Co0.5S/SN-TiO2 nano-fibers was higher than TiO2, CoS/SN-TiO2 and CdS/SN-TiO2 nano-fibers. The optimal 3-Cd0.5Co0.5S/SN-TiO2 with a Cd0.5Co0.5S ratio of 5.0 wt% performed the highest photocatalytic activity (4.55 mmol g?1 h?1), and the best photocatalytic durability after five cycles. It's owing to the hybrid effect of CdS and CoS for efficient transfer and separation of charge carriers at the junction interface between Cd0.5Co0.5S nanoparticles and S,N-codoped TiO2 nanofibers. Meanwhile, the extending visible-light response and sufficient active sites of TiO2-based heterojunctions are favorable for the water splitting.  相似文献   

20.
A novel nano-heterojunction photocatalysts of CdS/MoS2 with appropriate interfacial contact was successfully obtained by the facile two-step hydrothermal synthesis. The MoS2 ultrathin layer was well combined with CdS nanosheets and formed the interaction, which facilitated the transfer and separation of charges. The CdS/MoS2 15 wt% possessed much higher H2 evolution photocatalytic performance (35.24 mmol h?1 g?1), exhibiting an 85.95 times enhancement as compared to that of pure CdS (0.41 mmol h?1 g?1). Moreover, the photochemical stability of CdS/MoS2 heterojunctions was excellent, which showed no significant decrease in activity after four cycles of experiments. The finding provides a novel method to integrate the structure of MoS2 with CdS, which exhibits great potential in solar energy conversion.  相似文献   

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