Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 13
·3116-3121
·
IF 5.6
Xinyue Wang,Yibin Wang,Xinzhi Ma,Lingling Xu,Sirui Liu,Wei Wang,Huiqing Lu,Lili Wu
Cobalt diselenide (CoSe2) is considered a promising catalyst for hydrogen evolution reaction (HER); however, the limited active number, agglomeration, and quick deactivation by acid etching hinder its broad adoption. Herein, we report carbon layer-covered CoSe2 nanowire arrays grown on carbon cloth (C@CoSe2/CC). The structure of the nanowire array demonstrates synergistic effects in promoting the infiltration of electrolytes, accelerating the diffusion of H2 bubbles, and preventing CoSe2 from being etched by the electrolyte. Consequently, the overpotential and Tafel slope (193 mV, 54.3 mV dec−1) obtained sustained 24 h with a negligible overpotential deterioration. This study provides insights into optimizing the intrinsic activity of active sites.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2023
·Vol. 26
·期 24
·e202300303
·
IF 2.3
Youyang Xie,Pengtao Sheng,Weili Li,Yanling Li,Songtian Li
Graphical By changing Cu/In molar ratios of Cu−In−Se QDs from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a remarkable red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants. in Cu−In−Se QDs, a significant red-shift occurred from 660 nm to 760 nm when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. These results confirmed the strong effect of the Cu/In and Zn/Cu molar ratios on the intrinsic and dopants states related-transition channels, including the band-edge, conduction band-intragap acceptor, as well as the donor-acceptor. The large structural tolerance of I–III–VI group quantum dots (QDs) to off-stoichiometry allows their photoluminescence properties to be adjusted via doping, thereby enabling application in different fields. However, the photophysical processes underlying their photoluminescence mechanism remain significantly unknown. In particular, the transition channels of CuInSe 2 QDs, which are altered by intrinsic and extrinsic intragap states, remain poorly reported. Herein, we investigated the photophysical processes associated with intragap states via electrochemical and optical techniques by using copper deficient Cu−In−Se QDs as well as Zn doped Cu−In−Se QDs. When the Cu/In molar ratios of Cu−In−Se QDs increased from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants in Cu−In−Se QDs, a significant red-shift occurred (from 660 nm to 760 nm) when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. The Gaussian deconvolution results of the photoluminescence spectra and the band gap derived from absorption spectra by fitting supported the fact that the optical transition channels are dependent on the Cu/In and Zn/Cu molar ratios. After the introduction of the Zn 2+ ions, the alloyed-resultant blue-shift of the emission spectra was observed, primarily due to the enlarged band gap; however, the radiative recombination of prominent intrinsic intragap states is still observed; and only a small proportion of the band-edge exciton undergoes recombination for the sample with low Zn content. Cyclic voltammetry measurements revealed well-defined extrinsic Zn Cu intragap states (Zn substitution on Cu sites) and intrinsic Cu x (x= 1+/2+) states in the band gap. The results presented here provide a better understanding of the varying effects of dopant on photoluminescence in terms of I–III–VI group QDs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xinsheng Tang,Xiong Liu,Fangfei Liu,Tursun Abdiryim,Ruxangul Jamal,Nawrzhan Serkjan,Shuyue Xie,Cong Xue,Qian Cheng
Pyro-phototronic effect plays an important role in improving the photodetection performance of ultraviolet (UV) photodetectors (PDs). Here, a novel pyro-phototronic effect between TiO 2 nanoarrays (TiO 2 NRs) and the conducting polymer poly(3,4-ethylenedioxy selenophene) (PEDOS) is applied to fabricate a self-powered UV PD with the enhanced photodetection ability. The self-powered p-n heterojunction UV PD is fabricated by a face-to-face hybrid of acid (HCl and H 2 SO 4 )-treated TiO 2 NRs with PEDOS. Interestingly, a pyro-phototronic effect is found between TiO 2 NRs/FTO and PEDOS/FTO, and the acid treatment of TiO 2 NRs can dramatically enhance the pyro-phototronic effect. H 2 SO 4 treatment can improve the p-n heterojunction, while HCl treatment can increase carrier concentration due to the introduction of surface oxygen vacancies on the surface of TiO 2 NRs. Under UV light illumination and 0 bias voltage, the rise time (T rise ) and fall time (T fall ) of UV PD from the face-to-face hybrid of PEDOS/FTO with TiO 2 (HCl)/FTO are 0.080 s and 0.079 s, while the responsivity (R) and detectivity (D*) are 58.706 mA/W and 3.627 × 10 11 Jones, respectively. The face-to-face fabrication of UV PDs and the matching of the energy levels between PEDOS and TiO 2 NRs cause the pyro-phototronic effect due to temperature change and pyroelectric effect of TiO 2 NRs under the UV light illumination. This work gives a new idea to generate pyro-phototronic effect between TiO 2 NRs and conducting polymers for application in UV PDs field.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xichen Liu,Jianghao Wang,Yating Zhang,Dongzhi Zhang
A high-performance hydrogen sulfide sensor is introduced in this paper. CuO/MoSe 2 nanocomposites were synthesized using a simple hydrothermal method , and the sensing properties of CuO/MoSe 2 composite films for H 2 S gas were investigated at 75 °C. The gas sensor test results revealed that the CuO/MoSe 2 composite membrane sensor outperforms the single material sensor in terms of response, response/recovery time, linearity, and long-term stability. The enhanced gas sensitivity of the CuO/MoSe 2 nanocomposite could be attributed to the synergistic effect of the two materials' p-p heterojunction . Using DFT simulation, it was also shown that the CuO/MoSe 2 composite sensor's ability to adsorb H 2 S is superior to that of CuO and MoSe 2 used alone.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 29
·15833-15843
·
IF 11.9
Yi Tao,Zikun Tang,Yihong Zhong,Dequan Bao,Zhenqiu Gao,Wei Zhao,Zhen Wen,Hao Zhang,Kanghong Wang,Xuhui Sun
Photoelectrochemical (PEC) water splitting is a promising approach for the conversion of solar energy to hydrogen fuel. However, the solar-to-hydrogen (STH) efficiency is still restricted by the kinetically sluggish oxidation reaction on the surface of the photoanode. Herein, a unique composite structure (ZnO@NiO–QDs) was developed as the photoanode, in which the highly dispersed ZnO (d-ZnO) particles derived from the pyrolysis of ZIF-8 serve as the scaffolds to support NiO (cocatalysts) and colloidal CdSe(CdSexS1−x)4(CdS)2 QDs (denoted as CAS, a light absorber). Due to the enhanced hole consumption accelerated by NiO cocatalysts, the optimized photoanode (d-ZnO@NiO0.03–CAS) exhibits a higher saturated current density (Jsc) of 21.7 mA cm−2 than the d-ZnO–CAS photoanode (15.6 mA cm−2) under standard one sun (AM 1.5 G, 100 mW cm−2) solar irradiation. More importantly, such an electrode can still work as an electrocatalyst under light-off conditions via a sole electrochemical (EC) process. Thus, a well-designed bifunctional electrode that integrates cocatalysts and light absorbers makes it possible to generate hydrogen efficiently under both light-on and light-off conditions, providing an efficient and low-cost paradigm to improve the hydrogen evolution performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Wenrui Wu,Yue Yan,Yingsong Yu,Xing Wang,Tao Xu,Xianfu Li
Transition metal selenides (TMSs) are viewed as a prospective high-capacity electrode material for asymmetric supercapacitors (ASCs). However, the inability to expose sufficient active sites due to the limitation of the area involved in the electrochemical reaction severely limits their inherent supercapacitive properties. Herein, a self-sacrificing template strategy is developed to prepare self-supported CuCoSe (CuCoSe@rGO-NF) nanosheet arrays by in situ construction of copper-cobalt bimetallic organic framework (CuCo-MOF) on rGO-modified nickel foam (rGO-NF) and rational design of Se 2- exchange process. Nanosheet arrays with high specific surface area are considered to be ideal platforms for accelerating electrolyte penetration and exposing rich electrochemical active sites. As a result, the CuCoSe@rGO-NF electrode delivers a high specific capacitance of 1521.6 F/g at 1 A/g, good rate performance and an excellent capacitance retention of 99.5% after 6000 cycles. The assembled ASC device has a high energy density of 19.8 Wh kg −1 at 750 W kg −1 and an ideal capacitance retention of 86.2% after 6000 cycles. This proposed strategy offers a viable strategy for designing and constructing electrode materials with superior energy storage performance.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Haorui Dong,Haiyan Zhao,Tongtong Xuan,Wenhao Bai,Tianyu Lin,Yixin Cai,Rong-Jun Xie
Lead halide perovskite nanocrystals (NCs) have been the star material in lighting and displays owing to their excellent photoelectrical properties, but they have not simultaneously realized high photoluminescence quantum yield (PLQY) and high stability. To solve this problem, we propose a perovskite/linear low-density polyethylene (perovskite/LLDPE) core/shell NC by the synergistic role of the pressure effect and steric effect. Green CsPbBr3/LLDPE core/shell NCs with near-unity PLQY and nonblinking behavior were synthesized through an in situ hot-injection process. The mechanism of the improved photoluminescence (PL) properties is the enhanced pressure effect resulting in increased radiative recombination and interaction between the ligand and perovskite crystals, as confirmed by the PL spectra and finite element calculations. Meanwhile, the NCs show high stability under ambient conditions (with a PLQY of 92.5% after 166 days) and against 365 nm UV light (maintaining 61.74% of the initial PL intensity after continuous radiation for 1000 min). This strategy also works well in the blue and red perovskite/LLDPE NCs and red InP/ZnSeS/ZnS/LLDPE NCs. Finally, white-emitting Mini-LEDs were fabricated by combining the green CsPbBr3/LLDPE and red CsPbBr1.2I1.8/LLDPE core/shell NCs with blue Mini-LED chips. The white-emitting Mini-LEDs exhibit super wide color gamut (∼129% of the National Television Standards Committee or 97% of the Rec. 2020 standards).
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ANALYTICAL SCIENCES
·
2023
·Vol. 39
·期 8
·1391-1403
·
IF 1.6
Zhu Leijing,Ma Jing,Jin Danli,Zhang Yongjian,Wu Siyu,Xu Ajing,Gu Yingying,An Yarui,Miao Yuqing
The abnormal concentrations of human immunoglobulin G (hIgG) refers to many kinds of diseases. Analytical methods with the characteristics of rapid response, easy operation and high sensitivity should be designed to accurately determinate the hIgG levels in human serum. In this work, a label-free electrochemical immunosensor based on WSe 2 /rGO was developed to sensitively detect human immunoglobulin G. First, the flower-like transition metal dichalcogenides (TMDCs) Tungsten Diselenide (WSe 2 ) with large effective specific surface area and porous structure was synthesized by hydrothermal synthesis. As a bio-matrix, the flower-like WSe 2 efficiently increased the active sites for loading antibodies. Meanwhile, reduced graphene oxide (rGO) obtained by tannic acid reduction was used to improve the current response of the sensing interface. WSe 2 was combined with rGO and the electrochemical active surface area (ECSA) of the sensing interface was enlarged to 2.1 times that of GCE. Finally, the combination of flower-like WSe 2 and rGO broadened the detection range and reduced the detection limit of the sensing platform. The immunosensor exhibited a high sensitivity with a wide linear range of 0.01–1000 ng/mL and low detection limit of 4.72 pg/mL. The real sample analysis of hIgG were conducted under optimal conditions, and the spiked recovery rates were between 95.5 and 104.1%. Moreover, satisfactory results were obtained by testing the stability, specificity and reproducibility of the immunosensor. Therefore, it can be concluded that the as-proposed immunosensor has the application potential of clinical analyze of hIgG in human serum. Graphical abstract
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FIBERS AND POLYMERS
·
2023
·Vol. 24
·期 6
·1903-1917
·
IF 2.5
Tian Qianjun,Huang Zhichao,Wang Lin,Shi Lei,Shen Liangen,Qi Dongming
Self-healing polyurethane materials with excellent mechanical properties have a wide range of applications, including textiles, clothing, leather, and flexible electronics. However, determining methods to obtain this material in green and environment-friendly ways is an interesting and challenging task. In this study, a series of self-healing polyurethane materials with soft segments containing diselenide bonds and hard segments including multiple hydrogen bonds were prepared using a solvent-free method. The characterization results demonstrated that the T–Se–SFPU–2 sample exhibited both favorable self-healing function as well as mechanical properties with a tensile breaking strength of 6.15 MPa, and the greatest healing effect was achieved after 6 h at room temperature under visible light. The research results further demonstrated that the hydrogen bond in the hard segment can considerably improve the mechanical properties of polyurethane. The best micro-phase separation was achieved by controlling the hydrogen bond content in the hard segment, achieving a force balance between the soft and hard segments, and finally, the optimal balance between the self-healing performance and mechanical strength of polyurethane was achieved. These results provide a new strategy for preparing polymers with different self-healing capabilities.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Haonan Wang,Kaifeng Yu,Pengtao Wang,Pengcheng Jia,Yongzhi Yuan,Ce Liang
Metal-organic frameworks (MOFs) have the advantages of controllable chemical properties, rich pore structures and reaction sites and are expected to be high-performance anode materials for the next generation of potassium-ion batteries (PIBs). However, due to the large radius of potassium ions, the pure MOF crystal structure is prone to collapse during ion insertion and processing, so its electrochemical performance is quite limited. In this work, a hollow carbon sphere-supported MOF-derived Co/CoSe heterojunction anode material for potassium-ion batteries was developed by a hydrothermal method . The anode has high potassium storage capacity (461.9 mA h/g after 200 cycles at 1 A/g), excellent cycling stability and superior rate performance. It is worth noting that the potassium ion storage capacity of the anode material shows a gradual upward trend with the charge–discharge cycle, which is 145.9 mA h/g after 3000 cycles at a current density of 10 A/g. This work demonstrates that MOF-derived CoSe anodes with high capacity and low cost may be promising candidates for the introduction of potassium ion storage.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiang Shang,Yong Jin,Weining Du,Long Bai,Rong Zhou,Wenhua Zeng,Kunyan Lin
Waterborne polyurethane has drawn extensive attention due to its environmental friendliness and is widely used in many areas. However, it is still a great challenge to synthesize waterborne polyurethanes with flame retardancy and fast room-temperature self-healing ability, along with excellent mechanical performance and emulsion stability due to the mutually contradictory nature of these properties. Herein, waterborne polyurethanes containing organic selenium (SWPU-x) from 0.67 to 3.28 wt % were synthesized, which could simultaneously realize flame retardancy and self-healing ability based on the ability to scavenge active free radicals at high temperature and the dynamic switch of diselenide. All these SWPU-x films self-extinguished within 1 s after the ignition in the vertical combustion tests. The limiting oxygen index of SWPU-4 was improved to 28.5% with excellent UL-94 level (V-0) and self-healing efficiency (91.25%, after being healed in the photoreactor for 30 min at room temperature), together with high mechanical properties (tensile strength was 18.5 MPa and elongation at break was 869.63%), and the total heat release (THR) for SWPU-4 (49.28 MJ/m2) could decrease to 23.80% of the THR for the original waterborne polyurethane WPU (64.67 MJ/m2). This work discovered a new flame-retardant element (organic selenium) and studied its flame-retardant behaviors and self-healing function simultaneously, which would extremely extend the application of waterborne polyurethanes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Deng Long,Jia Liu,Hongyu Chen,Pei Liu,Kai Zheng,Yibo Zeng,Xinyi Chen,Shuang Li,Miao Lu
How to passivate the recombination in a photocatalyst is a big challenge to achieve efficient photocatalytic CO 2 reduction. Besides the heterojunction strategy, the design of intrinsic built-in electric field in a single phased photocatalyst can facilitate the transport while it does not introduce extra side reactions induced by the unbalanced photocarriers. This work utilizes the electronegative diversity between chalcogens and non-chalcogen element in a quarternary transition metal dichalcogenide of MoS x Se y N z to define localized built-in electric fields. It has been revealed that the nitrogen induced intrinsic dipole moments and potential energy have strenghthened the built-in electric fields, promoting the separation of photocarriers and the gathering of electrons around N sites, which has been found to improve the adsorption of intermediate products and lower the energy for methanol-oriented photoproduction route. Finally, the MoS x Se y N z has improved the photoproduction of methanol reduced from CO 2 by 162%.
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