Nanoscale
·
2020
·Vol. 12
·期 20
·11267-11279
·
IF 6.895
Hongkai Zhao,Xiaoxia Li,Mingyue Zheng,Xian Zhao,Qun Zhang,Yi Luo,Weiliu Fan
The construction of both highly efficient and stable hybrid artificial photosynthetic systems comprising semiconductors as photosensitizers and abundant metal-based molecular complexes as cocatalysts for photocatalytic H2 generation remains challenging. Herein, we report an effective and stable CdS/cobaloxime hybrid system prepared by inserting an amorphous TiO2 (a-TiO2) interlayer with adjustable thickness and by covalently-surface-attaching molecular cobaloxime catalysts. This hybrid system displayed outstanding photocatalytic H2 production and reached a maximum rate of ∼25 mmol g−1 h−1, which was ∼20.8 times that of pure CdS and 1.7 times that of the CdS/cobaloxime system without an a-TiO2 interlayer (CdS/Co). More importantly, 6 nm a-TiO2 uniformly coated CdS nanorods (CdS NRs) exhibited exceptional 200 h long-term catalytic behaviour under ≥420 nm visible light irradiation. However, the H2 production performance of the CdS/Co hybrid system decreased significantly over 10 h. Density functional theory (DFT) calculations indicated that the a-TiO2 surface can provide abundant bonding sites for the effective immobilization of molecular catalysts. Moreover, Mott–Schottky electrochemical measurements and femtosecond transient absorption spectroscopy revealed that the a-TiO2 interlayer had favourable band levels that could fasten the photoexcited electron transfer from CdS to molecular cobaloxime and could extract holes with intraband electronic states generated by defects, thus prohibiting CdS photocorrosion and improving the stability of the hybrid system. This study proposes a strategy for designing multifunctional interlayers for the effective immobilization of molecular catalysts, beneficial regulation of photoinduced charge carriers, and improvement of the stability as well as facilitation of the construction of artificial photosynthetic hybrid systems with high efficiency and durability.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Taiping Hu,Kai Dai,Jinfeng Zhang,Guangping Zhu,Changhao Liang
Inorganic-organic hybrid materials, a class of probable candidates for combining two counterparts into one structure could be beneficial for improving or combing the excellent electronic, magnetic, rigidity and thermal stability, and optical feathers of inorganic frameworks with diverse structure, processability, flexibility and good geometric controllability of organic molecules. Anchoring inorganic-organic hybrid materials with cocatalysts is a usually used strategy for enhancing their catalytic performance. However, noble metal cocatalysts always limit their practical application. Herein, we report that noble metal free cocatalyst of Ni 2 P decorated CdS-diethylenetriamine (CdS-DETA) can effectively overcome this limitation to achieve highly photocatalytic hydrogen production . The rapid microwave solvothermal synthesis of CdS-DETA (MCdS-DETA) process shortens reaction time, saves energy and lead to achieve highly photocatalytic activity due to its low crystallinity . When Ni 2 P decorated MCdS-DETA, The 0.4%Ni 2 P/MCdS-DETA exhibited the highest photocatalytic hydrogen evolution activity (6836 μmmol h −1 g −1 ), which is 4.14 times, 2.06 times and 1.34 times higher than traditional solvothermal CdS-DETA(TCdS-DETA), MCdS-DETA and Pt cocatalysted MCdS-DETA, respectively. The method reported here can be extended to other inorganic-organic hybrid materials, and develops new strategies for exploring inorganic-organic hybrid-based photocatalysts .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Weiwei Han,Lulu Chen,Weiyu Song,Shaobin Wang,Xiaobin Fan,Yang Li,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Nitrogen and sulfur co-doped reduced graphene oxide (NS-rGO) was synthesized using a facile low temperature calcination method, which was then used as support and cocatalyst for the anchor of CdS. The obtained CdS/NS-rGO nanocomposites exhibit ultra-high photocatalytic activity for hydrogen evolution and 4-nitrophenol (4-NP) reduction under visible light (λ ≥ 420 nm). Their activity could also be adjusted by changing the doping amount of S and N, or by changing the ratios between CdS and NS-rGO. The optimum percentage of NS-rGO is 5 wt%, at which CdS/NS-rGO photocatalyst could achieve the highest H 2 evolution rate of 1701 μmol h –1 g –1 . Moreover, the reduction from 4-NP to 4-aminophenol (4-AP) could be completed within only 6 min over this optimized composite. NS-rGO here could provide more active sites as well as tune the band gap structure to increase the photo-activity. The density functional theory (DFT) calculations reveal that NS-rGO has a small Gibbs free energy for H* adsorption (Δ G H ), which could increase the utilization efficency of photo-generated electrons for H 2 generation. NS-rGO is therefore an idea alternate cocatalyst of noble metals for new photocatalysts development.
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高影响因子
OPTICAL MATERIALS
·
2018
·
IF 2.32
Cheng Zhao,Xu Zhang,Xiaoqing Shu,Xudong Liu,Dawei Fang,Youtao Song,Jun Wang
In this paper, Er-doped carbon quantum dots (Er-CQDs) is first incorporated into CdS quantum dot sensitized solar cells (QDSSCs) for broadening light absorption range and accelerating electron transport . Er-CQDs are prepared by hydrothermal method forming Er-CQDs/TiO 2 film. The CdS quantum dots (QDs) are deposited on Er-CQDs/TiO 2 film by successive ionic layer adsorption and reaction (SILAR) method, constituting CdS/Er-CQDs/TiO 2 photoanode . The structural and optical properties of the CQDs and CdS/Er-CQDs/TiO 2 photoanode are characterized by FT-IR, UV–vis, FL and PL techniques. The composition and morphology are confirmed by XRD , EDX, SEM and TEM techniques. The optical properties of the influence of Er-CQDs on photovoltaic performance of CdS QDSSCs is studied by electrochemical methods. The experiment data show that the photovoltaic performance of CdS/Er-CQDs/TiO 2 working electrode can greatly be enhanced compared that of CdS/TiO 2 . In comparison, the PCE increases from 0.34% of CdS/TiO 2 device to 0.43% of CdS/CQDs/TiO 2 device, whose escalating rate is 26.45%. Furthermore, the PCE increases from 0.34% of CdS/TiO 2 device to 0.59% of CdS/Er-CQDs/TiO 2 device, whose escalating rate reaches 73.53%.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Dandan Ma,Jian-Wen Shi,Diankun Sun,Yajun Zou,Linhao Cheng,Chi He,Zeyan Wang,Chunming Niu
Au nanoparticle (NP)- and CdS quantum dot (QD)-codecorated In2O3 nanosheets, assembled into flowerlike structure (In2O3/Au/CdS), were synthesized to facilitate photocatalytic H2 production. The optimized In2O3/Au4/CdS-12 (4 wt % Au NPs and CdS QDs were deposited for 12 cycles) displays achieved a photocatalytic hydrogen generation ability of 17.23 μmol/h (10 mg of catalyst), which is 22.97, 5.08, and 5.05 times as high as that of pristine In2O3 (0.75 μmol/h), In2O3/Au4 (3.39 μmol/h), and In2O3/CdS-12 (3.41 μmol/h), respectively. This significant improvement of H2 generation rate can be attributed to the following factors: the heterojunction at the In2O3–CdS interface and the Schottky barrier at the interface between In2O3–Au and CdS–Au improves the migration and separation of charge carriers, and the surface plasma resonance (SPR) effect of noble metal Au NPs enhances the light harvesting capacity of In2O3 and boosts the generation of hot electrons, efficiently improving the utilization rate of sunlight.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Pan Li,Xuehua Zhang,Chunchao Hou,Yong Chen,Tao He
Fabrication of hybrid system coupling inorganic semiconductor photosensitizer with molecular catalyst provides a promising approach to achieve highly efficient CO 2 reduction into solar fuels, as the semiconductor nanomaterials can meet the prerequisites of visible-light photoresponse and high charge-separation efficiency for achieving high photocatalytic efficiency. In this work, CdS/Bi 2 S 3 heterostructures have been prepared via an ion-exchange reaction and employed as the photosensitizer to couple with tetra(4-carboxyphenyl)porphyrin iron(III) chloride (FeTCPP) molecular catalyst for photoreduction of CO 2 into CO and H 2 under visible-light irradiation. The sulfur vacancy in CdS surface can be reduced by the formation of CdS/Bi 2 S 3 heterostructure. The content of Bi 2 S 3 can be modulated via tailoring the ion-exchange reaction time. The resulting effect on the performace of CO 2 photoreduction has been investigated in detail. Benefiting from the enhanced separation and utilization of charge carriers, CdS/Bi 2 S 3 -0.5 h/FeTCPP hybrid catalyst exhibits 8.2 times CO yield (1.93 mmol/g/h) and 1.7 times H 2 yield (6.08 mmol/g/h) of CdS/FeTCPP hybrid catalyst. More important, the results of energy level alignment, electron spin resonance and photocatalysis indicate that electron-transfer direction can be changed once the CdS/Bi 2 S 3 heterostructure is coupled with FeTCPP. In the CdS/Bi 2 S 3 heterostructure, electrons transfer mainly from the conduction band of CdS to Bi 2 S 3 , while it is mainly from the conduction band of CdS to FeTCPP in the CdS/Bi 2 S 3 /FeTCPP hybrid.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 21
·18059-18066
·
IF 2.324
Li Zhen,Yu Libo,Song Hai,Feng Lei,Wang Xingpeng
TiO 2 nanoparticles (NP) at top of TiO 2 nanotube (TiO 2 NP@TiO 2 NT) double-layered architecture is constructed to combine the advantages of TiO 2 NP and TiO 2 NT together. This composite TiO 2 NP@TiO 2 NT architecture as photoanode possesses a larger surface area for more QDs loading, and highly tubular structure for electron swift transport. Based on this architecture, CdSe/CdS quantum dots (QDs) have been successfully synthesized by successive ionic layer adsorption reaction (SILAR) method for quantum dots-sensitized solar cell application. The photovoltaic performance of QDSSCs based on TiO 2 NP@TiO 2 NT have been investigated in contrast with bare TiO 2 NP and bare TiO 2 NT architectures with almost the same thickness. The results show that the power conversion efficiency (PCE) of QDSSCs could be enhanced using TiO 2 NP@TiO 2 NT and improved to 3.26%, which is 80% and 38% higher than QDSSCs based on bare TiO 2 NT and bare TiO 2 NP, respectively. The BET surface area, UV–vis absorption spectra, and incident photon to current conversion efficiency (IPCE) measurements results show the evidence that the TiO 2 NP@TiO 2 NT can combine advantages of TiO 2 NP and TiO 2 NT structures together and lead to a higher light harvesting efficiency, electron collecting efficiency, and efficient electron transport.
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高影响因子
RSC Advances
·
2015
·Vol. 5
·期 86
·70345-70351
·
IF 3.84
Qingkun Kong,Meng Li,Chao Ma,Hongmei Yang,Shenguang Ge,Mei Yan,Jinghua Yu
A simple electrochemiluminescence (ECL) aptasensor for adenosine triphosphate (ATP) based on graphene/polyaniline (GR/PANI) composite films modified glassy carbon electrode (GCE) was successfully fabricated. The GR/PANI composite film using graphite oxide (GO) and aniline as the starting materials was obtained through a new one-step large-scale electrochemical synthesis for the immobilization of the first probe. PNNs could be synthesized through the chemical reduction of H2PtCl6 by benzyl alcohol under microwave irradiation without the introduction of any surfactants, templates, or seeds. PNNs@CdS QDs were used as an excellent label with amplification techniques. Taking advantage of dual-amplification effects, the aptasensor could detect ATP quantitatively, in the range from 0.5 pM to 20 nM, with a limit of detection as low as 0.1 pM. The proposed ECL aptasensor should have wide applications in the diagnosis of genetic diseases due to its simplicity, low cost, and high sensitivity at extremely low concentrations.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2015
·
IF 6.409
Ting Hou,Lianfang Zhang,Xinzhi Sun,Feng Li
Herein, we reported a facile and highly sensitive biphasic photoelectrochemical (PEC) sensing strategy based on enzymatic product-mediated in situ formation of CdS quantum dots (QDs), and assayed the activity and inhibition of acetylcholinesterase (AChE) in its optimal state. Upon the hydrolysis of acetylthiocholine catalyzed by AChE, the product thiocholine stabilizes the in situ formation of CdS QDs in homogenous solution. Due to the electrostatic attraction , the resulting tertiary amino group-functionalized CdS QDs are attached to the surface of the negatively charged indium tin oxide (ITO) electrode, generating significant PEC response upon illumination in the presence of electron donors . By taking full advantage of the in situ formation of CdS QDs in homogenous solution, this strategy is capable of detecting AChE activity and inhibition in its optimal state. A directly measured detection limit of 0.01 mU/mL for AChE activity is obtained, which is superior to those obtained by some fluorescence methods . The inhibition of AChE activity by aldicarb is successfully detected, and the corresponding IC 50 is determined to be 13 μg/L. In addition to high sensitivity and good selectivity, this strategy also exhibits additional advantages of simplicity, low cost and easy operation. To the best of our knowledge, the as-proposed strategy is the first example demonstrating the application of CdS QDs formed in situ for biphasic PEC detection of enzyme activity and inhibition. More significantly, it opens up a new horizon for the development of homogenous PEC sensing platforms, and has great potential in probing many other analytes.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2015
·
IF 2.711
Jian-Jian Zhou,Rong Wang,Xin-Ling Liu,Fu-Min Peng,Chuan-Hao Li,Fei Teng,Yu-Peng Yuan
CdS nanoparticles acting as photosensitizer was grown in situ upon UiO-66 metal-organic framework octahedrons through a hydrothermal process. The resultant CdS/UiO-66 hybrid photocatalysts show remarkably active hydrogen evolution under visible light irradiation as compared to CdS and UiO-66 alone. The optimum hybrid with 16 wt% CdS loading shows a hydrogen production rate of 235 μmol h −1 , corresponding to 1.2% quantum efficiency at 420 nm. The improved photocatalytic hydrogen production over hybrid CdS/UiO-66 is ascribed to the efficient interfacial charge transfer from CdS to UiO-66, which effectively suppresses the recombination of photogenerated electron-hole pairs and thereby enhancing the photocatalytic efficiency.
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高影响因子
FOOD CONTROL
·
2013
·
IF 2.738
Xianyi Cao,Fei Shen,Minwei Zhang,Jiajia Guo,Yeli Luo,Xing Li,Han Liu,Chunyan Sun,Jingbo Liu
A simple, rapid and ultra-sensitive analytical method for the determination of melamine in raw milk based on inner filter effect (IFE) of Au nanoparticles (AuNPs) on the fluorescence of CdS quantum dots (QDs) is described in this study. With the presence of citrate-stabilized AuNPs, the fluorescence of l -cysteine ( l -Cys)-capped CdS QDs was remarkably quenched by AuNPs via IFE. The fluorescence of the AuNPs-CdS QDs system was recovered upon addition of melamine, since melamine could induce the aggregation of AuNPs accompanying the reduction of their characteristic plasmon absorption at ∼522 nm, which resulted in “turn-on” of the IFE-decreased fluorescence of CdS QDs. Under the optimum conditions, a good linear correlation for detection of melamine in raw milk was exhibited from 0.05 mg·L −1 to 0.35 mg·L −1 , and the detection limit was 0.017 mg·L −1 , which was much lower than the detection limit of HPLC coupled with UV detector and the safety limit required by USA, UK and China. This method was successfully carried out for the assessment of melamine in raw milk samples, which revealed many advantages such as high sensitivity, low cost and non-time-consuming compared with traditional methods.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2015
·Vol. 40
·期 2
·1878-1881
·
IF 3.086
Yong Cui,Zhe Zhang,Xu Du,Wei Liu,Yulin Deng,Shi Liu,Gang Wang
CuIn0.9R0.1(S,Se)2 (R = Al, Ni, Co) thin films were obtained via a solution process based on homogeneous precursor solutions and selenization. The as-prepared thin films were characterized by XRD, EDS and SEM. The CdS buffer layer was deposited by a solution process on the CuIn0.9R0.1(S,Se)2 (R = Al, Ni, Co) thin films, and Mo/CuIn0.9R0.1(S,Se)2 (R = Al, Ni, Co)/CdS/i-ZnO/ITO/Al thin-film solar cells were fabricated. The efficiencies of the as-fabricated CuIn0.9R0.1(S,Se)2 (R = Al, Ni, Co) thin-film solar cells were 4.33%, 2.38% and 1.98%, respectively.
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高影响因子
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