Environmental Science-Nano
·
2020
·Vol. 7
·期 12
·3877-3887
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IF 7.683
Wanjun Wang,Wenquan Gu,Guiying Li,Haojing Xie,Po Keung Wong,Taicheng An
Sustainable and “green” technologies for hydrogen peroxide (H2O2) production have aroused increasing interest, yet challenges prevail in production of H2O2 for environmental applications. In this study, tungsten selenide (WSe2) with a few-layered microstructure was used as a new co-catalyst to synthesize H2O2 under visible light irradiation. The ultrathin WSe2 nanosheets were anchored onto a g-C3N4 surface by in situ growth solvothermal methods. The as-prepared WSe2/g-C3N4 showed remarkably enhanced H2O2 production efficiency without organic electron donors, which was 11.8 times higher than that of pristine g-C3N4. H2O2 was generated via O2 reduction mediated by photogenerated e−, and dissolved O2 could be generated by water oxidation and in situ used to produce H2O2 under anaerobic conditions. The introduction of WSe2 not only promoted visible light absorption, but also facilitated the charge transfer efficiency by forming a Z-scheme rather than a type II heterojunction. The photogenerated e− was enriched onto WSe2, leading to the high H2O2 production activity. Moreover, the in situ generated H2O2 could be directly used for pathogenic bacteria inactivation through Fenton reactions without external H2O2 addition. This work is expected to open an avenue for developing novel photocatalysts towards sustainable H2O2 production for water disinfection and related environmental applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Minglu Li,Chaozhu Shu,Anjun Hu,Jiabao Li,Yu Yan,Miao He,Jianping Long
Lithium-oxygen batteries (LOBs) are considered to be one of the most competitive energy storage devices due to their high theoretical energy density . However, challenges including poor catalytic activity and durability of the oxygen electrode seriously hinder the in-depth development of LOBs. Adjusting the surface electronic structure of the oxygen electrode provides a new prospect for realizing highly efficient electrocatalysts . In this contribution, we report that atomic-scale palladium (Pd) involving in MoSe 2 (Pd–MoSe 2 ) is capable of adjusting the in-plane electron density of MoSe 2 via spontaneous interface chemical reactions, thereby accelerating the electron migration along the in-plane direction. The synergy between the created Se vacancies and Pd atoms can further increase the electroactive sites on the Pd–MoSe 2 surface, which is conducive to improving the catalytic activity of the electrode and thereby accelerating the kinetics of oxygen electrode reactions. The results show that Pd–MoSe 2 based LOBs exhibit excellent electrochemical performance such as high Coulombic efficiency (97.81%) as well as extended cycle life (1952 h). This work shows that the adjustment of in-plane electron density by exotic metal atom is a viable strategy to improve the catalytic activity of layered transition metal selenide, which provides the possibility of developing highly efficient electrocatalysts for LOBs.
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NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 40
·17313-17322
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IF 3.288
Guigui Liu,Chao Shuai,Zunli Mo,Ruibin Guo,Nijuan Liu,Xiaohui Niu,Qibing Dong,Jia Wang,Qinqin Gao,Ying Chen,Wentong Liu
The design and preparation of highly efficient and durable non-noble metal electrocatalysts for overall water splitting is pivotal for actualizing large-scale water splitting via electrolysis. Herein, porous Ni0.85Se nanospheres anchored on reduced graphene oxide (RGO) (Ni0.85Se/RGO) were synthesized via a one-step hydrothermal method. Following explorations of the hydrothermal temperature and reaction time, the optimized Ni0.85Se/RGO exhibited extraordinary oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance in 1.0 M KOH solution, providing an overpotential as small as 320 mV at a current density of 30 mA cm−2 and a low Tafel slope of 91 mV dec−1 for the OER, and an overpotential of 169 mV at a current density of 10 mA cm−2 and a low Tafel slope of 65 mV dec−1 for the HER. A current density of 10 mA cm−2 at 1.64 V and high stability can be obtained upon using Ni0.85Se/RGO as both the cathode and anode for overall water splitting under alkaline conditions; this was attributed to the merits of both the porous structure of Ni0.85Se and the high conductivity of RGO. This work provides a meaningful exploration of the synthesis of 3d-transition-metal-chalcogenide- and carbon-based composite electrocatalysts via a hydrothermal reaction for water splitting, and provides a general method.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Lei Yang,Liutao Huang,Yihang Yao,Lifang Jiao
High-efficiency electrocatalysts for water splitting can be achieved by constructing heterostructure engineering purposely. The same pyrite structure of NiSe 2 /NiP 2 with admirable electrical conductivity of NiSe 2 and outstanding stability of NiP 2 is designed to boost electrocatalytic performance towards overall water splitting. Density functional theory (DFT) calculations identify that constructing NiP 2 /NiSe 2 heterointerfaces with good lattice matching and the redistribution of electron between the heterointerfacecan optimize adsorption/desorption energy of H* effectively. Therefore, NiP 2 /NiSe 2 heterostructure on carbon fiber cloth with one-step phosphoselenization is developed as electrocatalysts. As expected, NiP 2 /NiSe 2 exhibits excellent catalytic activity with only 160 mV overpotential to realize a current density of 100 mA cm −2 and exceptional stability over 90 h at the current density of 10 mA cm −2 for HER in alkaline solution. This heterostructure strategy might be a new break-through for modulating the single-phase transition metal and designing highly active and durable catalysts towards water splitting.
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Journal of Physical Chemistry C
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2021
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IF 4.126
Zhiwei Yao,Chenghao Bi,Jianjun Tian
Quantum dot light-emitting diodes (QLEDs) show great potential in high-definition displays due to their narrow emission and high color purity. However, the imperfect quantum dots (QDs) with high trap density are difficult to be removed from QD solution, which could cause serious nonradiative recombination, thereby suppressing the improvement of QLEDs. Here, we devise a novel chemical filtering strategy with a bidentate coordination to remove the imperfect QDs. The bidentate ligand of ethanolamine (EA) with an amidogen and a carboxyl was directly added into the CdSe/CdS/ZnS core/shell/shell QD solution. Then, uncoordinated sites such as S2– and Zn2+ on the surface of QDs were bonded with the amidogen and carboxyl of EA, respectively, resulting in aggregations of the imperfect QDs with high defect density, which were precipitated from the solution. As a result, the photoluminescence quantum yield (PLQY) of the filtered QD solution increased to 93% because of the decrease in trap density. The size distribution of QDs was also improved after filtration. QLEDs fabricated with filtered QDs show a high external quantum efficiency (EQE) of 15.76% and luminance of 19,640 cd/m2, greater than those of the control devices. This strategy shows a great potential to be used in the large-scale treatment and production of QDs and QLEDs.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 11
·2008453
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IF 18.808
Pai Liu,Yajun Lou,Shihao Ding,Wenda Zhang,Zhenghui Wu,Hongcheng Yang,Bing Xu,Kai Wang,Xiao Wei Sun
InP quantum dots (QDs) are emerging as promising materials for replacing cadmium-based QDs in view of their heavy metal-free and tunable luminescence. However, the development of InP QD materials still lags due to the expensive and flammable phosphorus precursors, and also the unsatisfactory repeatability caused by the fast nucleation rate. Adopting lowly reactive P precursor aminophosphine can overcome this issue, but their low photoluminescence quantum yield (PLQY) and widening line widths do not apply to the practical application. Through engineering, the core-shell structure of QD, significantly promoted green emissions of QDs were obtained with PLQY of 95% and full width and half maximum (FWHM) of 45 nm, which demonstrated the highest PLQY record obtained from the aminophosphine system. Moreover, due to the residue halogen atoms on the QD surface as inorganic ligands to prevent further oxidization, these InP QDs demonstrated the ultra-long operational lifetime (over 1000 h) for QDs based color enhancement film. By optimizing the device structure, an inverted green InP quantum dot light-emitting diode (QLED) with external quantum efficiency (EQE) of 7.06% was also demonstrated, which showed a significant promise of these InP QDs in highly effective optoelectronic devices.
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
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2021
·Vol. 54
·期 11
·115504
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IF 3.207
Xi-Kai Yang,Jia-Wei Qiao,Zhi-Hao Chen,Zhen-Chuan Wen,Hang Yin,Xiao-Tao Hao
We adopt inorganic semiconducting CdSe quantum dots (QDs) as a third component in the PTB7-Th:PC71BM-based organic solar cells due to their advantages of strong absorbance, high conductivity, and good solution processability. With the blending of low-dosage CdSe QDs, the short-circuit current density (Jsc) and power conversion efficiencies can be improved by 13% and 11%, respectively, in the ternary device. Compared with the control device, CdSe QDs can effectively modulate the charge dynamics and lead to enhanced fluorescence external quantum efficiency. Moreover, effective Förster resonance energy transfer and fast charge transfer can be observed in the CdSe QD-based bulk-heterojunction (BHJ) films, and therefore improve the overall performance of the organic photovoltaic devices. This work provides an effective method by adopting CdSe QDs to fabricate high-performance PTB7-Th:PC71BM BHJ solar cells.
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NANO
·
2020
·
IF 1.566
Weili Li,Hongchao Geng,Lu Yao,Haiyan Xu,Yongjun Han,Pengtao Sheng
Oil phase CuInSe 2 quantum dots (CISe QDs) were synthesized via a hot-injection method, exhibiting a near-infrared (NIR) emission wavelength of 710 nm with poor fluorescence intensity. Therefore, we address this challenge by introducing two strategies: doping and ligand exchange. First, Zn was used as a dopant to improve the fluorescent properties of CISe QDs synthesized by the same method. The PL peak position of the resulting Zn–CuInSe (ZnCISe) QDs could be tuned from 600 nm to 662 nm, and the PL intensity of the QDs was greatly improved. Except that, this Zn doping strategy can help to improve the fluorescence lifetime and reduce defects, leading to increased quantum yield. Next, the aqueous phase transfer of ZnCISe QDs was achieved through an efficient ligand exchange strategy using glutathione (GSH) as the bifunctional ligand. Mercaptoacetic acid (MPA) was also used as an essential additive for GSH ligand exchange. With this method, we obtained high-quality hydrophilic ZnCISe QDs with particle sizes less than 3 nm and good monodispersity. In addition, DLS measurements showed a unimodal peak shape of the hydrated ZnCISe QDs in ultrapure water with particle sizes ranging from 7 nm to 40 nm. Finally, the cytotoxicity studies revealed that the viabilities of the cells incubated with ZnCISe QDs from 1 μ g/mL to 18 μ g/mL remained at levels greater than 90%, which indicates that QDs with good biocompatibility are promising fluorescent probes.
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Small
·
2020
·Vol. 16
·期 48
·2004457
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IF 11.459
Cai Liu,Miaoxin Zhang,Xin Zhang,Biao Wan,Xiaona Li,Huiyang Gou,Yexin Wang,Fuxing Yin,Gongkai Wang
Nano heterostructures relying on their versatile construction and the breadth of combined functionality have shown great potential in energy storage fields. Herein, 2D sandwiched MoSe 2 /TiO 2− x /graphene nano heterostructures are designed by integrating structural and functional effects of each component, aiming to address the rate capability and cyclic stability of MoSe 2 for sodium ion capacitors (SICs). These 2D nano heterostructures based on graphene platform can facilitate the interfacial electron transport, giving rise to fast reaction kinetics. Meanwhile, the 2D open structure induces a large extent of surface capacitive contribution, eventually leading to a high rate capability (415.2 mAh g −1 @ 5 A g −1 ). An ultrathin oxygen deficient TiO 2− x layer sandwiched in these nano heterostructures provides a strong chemical-anchoring regarding the products generated during the sodiation/desodiation process, securing the entire cyclic stability. The associated sodiation/desodiation mechanism is revealed by operando and ex situ characterizations, which exhibits a strong solid electrolyte interphase (SEI) dependence. The simulations verify the dependent sodiation products and enhanced heterostructural chemical-anchoring. Assembled SICs based on these nano heterostructures anode exhibit high initial Coulombic efficiency, energy/power densities, and long cycle life, shedding new light on the design of nano heterostructure electrodes for high performance energy storage application.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
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IF 3.807
KaiBo Zhang,XiaoBing Jiang,Min Zeng,Bo Jing
Lithium-ion batteries have progressively taken the place of conventional power sources and been extensively employed in our daily lives. In this study, a simple hydrothermal method was adopted to develop the two-dimensional layered MoSe 2 into three-dimensional porous microspheres and nanosphere structures hydrangea-like via directional polymerization, self-assembly and Ostwald maturation. Subsequently, the dopamine hydrochloride was polymerized and carbonized to modify the curd-shaped MoSe 2 by N-doped carbon coating. The modified MoSe 2 @N-C anode material exhibited a larger specific capacity, better stability and a higher rate at high current density than MoSe 2 anode material. The modified negative electrode material achieved the specific capacity of 553 mAh/g at a current density of 1 A/g and 300.8 mAh/g at 10 A/g. Under high current density, the long-cycle charge-discharge performance test was performed, and the modified material exhibited a significantly large specific capacity and high stability performance. Its electrochemical performance was enhanced due to the N-doped carbon coating layer on the surface that increased the material conductivity and reduced the shuttle effect of polyselenide.
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ChemSusChem
·
2021
·Vol. 14
·期 7
·1710-1719
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IF 8.928
Liwei Shi,Hailiang Fang,Xiaoxia Yang,Jie Xue,Caifeng Li,Shifeng Hou,Cheng Hu
Graphical Doping for batteries : Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates provide elevated performance as Li−S free-standing cathodes. Fe-doping in NiSe 2 enables improved charge transfer and stronger interactions with the adsorbed sulfur species, as well as higher electrical conductivity. The transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles eliminates the barriers of phase transitions during the cathode redox processes. The commercialization of Li−S batteries is hindered by the shuttling of lithium polysulfides (LiPSs), the sluggish sulfur redox kinetics as well as the low sulfur utilization during charge/discharge processes. Herein, a free-standing cathode material was developed, based on Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates (Fe-NiSe 2 /ACC) for high-performance Li−S batteries. Fe-doping in NiSe 2 plays a key role in the electronic structure modulation of NiSe 2 , enabling improved charge transfer with the adsorbed LiPSs molecules, stronger interactions with the active sulfur species and higher electrical conductivity. Effective promotion of the sulfur redox kinetics and enhanced sulfur utilization were achieved under high areal sulfur loadings. The stronger interactions with LiPSs together with the unique 3D structure of Fe-NiSe 2 /ACC also induced the transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles, significantly eliminating the barriers of solid nucleation and growth during the phase transition of liquid LiPSs to solid Li 2 S 2 /Li 2 S. With a high sulfur loading of 9.9 mg cm −2 , the Fe-NiSe 2 /ACC cathode enabled a high area capacity of 9.14 mAh cm −2 with a low average decay of 0.11 % per cycle over 200 cycles at 0.1 C.
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Nanoscale
·
2020
·Vol. 12
·期 45
·23013-23027
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IF 6.895
Ziqian Wang,Chenyue Zhan,Fang Zeng,Shuizhu Wu
Rheumatoid arthritis (RA) is a common chronic autoimmune disease associated with progressive disability, systemic complications, and poor prognosis. The improved understanding of the roles of immune signaling pathway inhibitors has shed light on designing new and more effective approaches for RA treatment. In this work, an inflammation-responsive and molecularly targeted drug system has been developed for RA therapy. The drug carrier was synthesized by covalently grafting hydrophobic cholesterol (Chol) molecules onto a hydrophilic chondroitin sulfate (CS) chain via the inflammation-responsive diselenide bonds (SeSe). The resultant amphiphilic polymer CSSeSeChol readily forms nanoparticles (NPs) and encapsulates two kinase inhibitors tofacitinib and SP600125 in aqueous media. Upon administration into the RA mouse model, the nanodrug accumulates in RA lesions and releases the inhibitors for regulating the JAK-STAT and JNK pathways. As a result, the nanodrug exhibits satisfactory efficacy in RA treatment by suppressing the expression of relevant pro-inflammatory cytokines, blocking the activation of osteoclasts and providing protection for cartilage and joints.
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