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991.
Songshan Bi Huimin Wang Yanyu Zhang Min Yang Qingjie Li Jinlei Tian Prof. Zhiqiang Niu 《Angewandte Chemie (International ed. in English)》2023,62(49):e202312982
Iodine (I2) shows great promising as the active material in aqueous batteries due to its distinctive merits of high abundance in ocean and low cost. However, in conventional aqueous I2-based batteries, the energy storage mechanism of I−/I2 conversion is only two-electron redox reaction, limiting their energy density. Herein, six-electron redox chemistry of I2 electrodes is achieved via the synergistic effect of redox-ion charge-carriers and halide ions in electrolytes. The redox-active Cu2+ ions in electrolytes induce the conversion between Cu2+ ions and I2 to CuI at low potential. Simultaneously, the Cl− ions in electrolytes activate the I2/ICl redox couple at high potential. As a result, in our case, I2-based battery system with six-electron redox is developed. Such energy storage mechanism with six-electron redox leads to high discharge potential and capacity, excellent rate capability, as well as stable cycling behavior of I2 electrodes. Impressively, six-electron-redox I2 cathodes can match various aqueous metal (e.g. Zn, Mn and Fe) anodes to construct metal||I2 hybrid batteries. These hybrid batteries not only deliver enhanced capacities, but also exhibit higher operate voltages, which contributes to superior energy densities. Therefore, this work broadens the horizon for the design of high-energy aqueous I2-based batteries. 相似文献
992.
Dr. Can Guo Jie Zhou Yuting Chen Huifen Zhuang Jie Li Jianlin Huang Yuluan Zhang Prof. Yifa Chen Prof. Shun-Li Li Prof. Ya-Qian Lan 《Angewandte Chemie (International ed. in English)》2023,62(11):e202300125
The inhomogeneous consumption of anions and direct contact between electrolyte and anode during the Zn-deposition process generate Zn-dendrites and side reactions that can aggravate the space-charge effect to hinder the practical implementation of zinc-metal batteries (ZMBs). Herein, electrospray has been applied for the scalable fabrication (>10 000 cm2 in a batch-experiment) of hetero-metallic cluster covalent-organic-frameworks (MCOF-Ti6Cu3) nanosheet-coating (MNC) with integrated micro space electrostatic field for ZMBs anode protection. The MNC@Zn symmetric cell presents ultralow overpotential (≈72.8 mV) over 10 000 cycles at 1 mAh cm−2 with 20 mA cm−2, which is superior to bare Zn and state-of-the-art porous crystalline materials. Theoretical calculations reveal that MNC with integrated micro space electrostatic field can facilitate the deposition-kinetic and homogenize the electric field of anode to significantly promote the lifespan of ZMBs. 相似文献
993.
Ruochen Zhang Dr. Yang Feng Dr. Youxuan Ni Beidou Zhong Maoyu Peng Dr. Tianjiang Sun Dr. Shan Chen Prof. Huan Wang Prof. Zhanliang Tao Prof. Kai Zhang 《Angewandte Chemie (International ed. in English)》2023,62(25):e202304503
Aqueous zinc batteries (AZBs) feature high safety and low cost, but intricate anodic side reactions and dendrite growth severely restrict their commercialization. Herein, ethylenediaminetetraacetic acid (EDTA) grafted metal organic framework (MOF-E) is proposed as a dually-functional anodic interphase for sustainable Zn anode. Specifically, the target-distributed EDTA serves as an ion-trapped tentacle to accelerate the desolvation and ionic transport by powerful chemical coordination, while the MOFs offer suitable ionic channels to induce oriented deposition. As a result, MOF-E interphase fundamentally suppresses side reactions and guides horizontally arranged Zn deposition with (002) preferred orientations. The Zn|MOF-E@Cu cell exhibits a markedly improved Coulombic efficiency of 99.7 % over 2500 cycles, and the MOF-E@Zn|KVOH (KV12O30-y ⋅ nH2O) cell yields a steady circulation of 5000 cycles@90.47 % at 8 A g−1. 相似文献
994.
Zn(II) ions sorption onto N‐Benzoyl‐N‐Phenylhydroxylamine (BPHA) impregnated polyurethane foam (PUF) has been studied extensively using radiotracer and batch techniques. Maximum sorption (~98%) of Zn(II) ions (8.9 × 10?6 M) onto sorbent surface is achieved from a buffer of pH 8 solution in 30 minutes using 7.5 mg/mL of BPHA‐impregnated polyurethane foam at 283 K. The sorption data follow Langmuir, Freundlich and Dubinin‐Radushkevich (D‐R) isotherms. The Langmuir constants Q = 18.01 ± 0.38 μ mole g?1 and b = (5.39 ± 0.98) × 103 L mole?1 have been computed. Freundlich constants 1/n = 0.29 ± 0.01 and Cm = 111.22 ± 12.3 μ mole g?1 have been estimated. Sorption capacity 31.42 ± 1.62 μ mole g?1, β = ?0.00269 ± 0.00012 kJ2 mole?2 and energy 13.34 ± 0.03 kJ mole?1 have been evaluated using D‐R isotherm. The variation of sorption with temperature yields ΔH = ?77.7 ± 2.8 k J mole?1, ΔS = ?237.7 ± 9.3 J mole?1 K?1 and ΔG = ?661.8 ± 117.5 k J mol?1 at 298 K reflecting the exothermic and spontaneous nature of sorption. Cations like Fe(III), Ce(III), Al(III), Pb(II) and Hg(II) and anions, i.e., oxalate, EDTA and tartrate, reduce the sorption significantly, while iodide and thiocyanate enhanced the sorption of Zn(II) ions onto BPHA‐impregnated polyurethane foam. 相似文献
995.
Luis A. García Rodenas Miguel A. Blesa Pedro J. Morando 《Journal of solid state chemistry》2008,181(9):2350-2358
Dissolution rates of NiO, CoO, ZnO, α-Fe2O3 and the corresponding ferrites in 0.1 mol dm−3 oxalic acid at pH 3.5 were measured at 70 °C. The dissolution of simple oxides proceeds through the formation of surface metal oxalate complexes, followed by the transfer of surface complexes (rate-determining step). At constant pH, oxalate concentration and temperature, the trend in the first-order rate constant for the transfer of the surface complexes (kMe; Me=Ni, Co, Zn, Fe) parallels that of water exchange in the dissolved metal ions (k−w). Thus, the most important factor determining the rates of dissolution of metal oxides is the lability of Me-O bonds, which is in turn defined by the electronic structure of the metal ion and its charge/radius ratio. UV (384 nm) irradiation does not increase significantly the dissolution rates of NiO, CoO and ZnO, whereas hematite is highly sensitive to UV light. For ferrites, the reactivity order is ZnFe2O4>CoFe2O4?NiFe2O4. Dissolution is congruent, with rates intermediate between those of the constituent oxides, Fe2O3 and MO (M=Co, Ni, Zn), reflecting the behavior of very thin leached layers with little Zn and Co, but appreciable amounts of Ni. The more robust Ni2+ labilizes less the corresponding ferrite. The correlation between log kM and log k−w is somewhat blurred and displaced to lower kM values. Fe(II), either photogenerated or added as salt, enhances the rate of Fe(III) phase transfer. A simple reaction mechanism is used to interpret the data. 相似文献
996.
Anisotropic Growth of Nonlayered CdS on MoS2 Monolayer for Functional Vertical Heterostructures 下载免费PDF全文
Wei Zheng Wei Feng Xin Zhang Xiaoshuang Chen Guangbo Liu Yunfeng Qiu Tawfique Hasan Pingheng Tan Ping An Hu 《Advanced functional materials》2016,26(16):2648-2654
2D semiconductors have emerged as a crucial material for use in next‐generation optotelectronics. Similar to microelectronic devices, 2D vertical heterostructures will most likely be the elemental components for future nanoscale electronics and optotelectronics. To date, the components of mostly reported 2D van der Waals heterostructures are restricted to layer crystals. In this work, it is demonstrated that nonlayered semiconductors of CdS can be epitaxially grown on to 2D layered MoS2 substrate to form a new quasi vertical heterostructure with clean interface by chemical vapor deposition. Photodetectors based on this CdS/MoS2 heterostructure show broader wavelength response and ≈50‐fold improvement in photoresponsivity, compared to the devices fabricated from MoS2 monolayer only. This research opens up a way to fabricate a variety of functional quasi heterostructures from nonlayered semiconductors. 相似文献
997.
Size Effects of Platinum Nanoparticles in the Photocatalytic Hydrogen Production Over 3D Mesoporous Networks of CdS and Pt Nanojunctions 下载免费PDF全文
Ioannis Vamvasakis Bin Liu Gerasimos S. Armatas 《Advanced functional materials》2016,26(44):8062-8071
Catalysts for the photogeneration of hydrogen from water are key for realizing solar energy conversion. Despite tremendous efforts, developing hydrogen evolution catalysts with high activity and long‐term stability remains a daunting challenge. Herein, the design and fabrication of mesoporous Pt‐decorated CdS nanocrystal assemblies (NCAs) are reported, and their excellent performance for the photocatalytic hydrogen production is demonstrated. These materials comprise varying particle size of Pt (ranging from 1.8 to 3.3 nm) and exhibit 3D nanoscale pore structure within the assembled network. Photocatalytic measurements coupled with UV–vis/NIR optical absorption, photoluminescence, and electrochemical impedance spectroscopy studies suggest that the performance enhancement of these catalytic systems arises from the efficient hole transport at the CdS/electrolyte interface and interparticle Pt/CdS electron‐transfer process as a result of the deposition of Pt. It is found that the Pt‐CdS NCAs catalyst at 5 wt% Pt loading content exerts a 1.2 mmol h?1 H2‐evolution rate under visible‐light irradiation (λ ≥ 420 nm) with an apparent quantum yield of over 70% at wavelength λ = 420 nm in alkaline solution (5 m NaOH), using ethanol (10% v/v) as sacrificial agent. This activity far exceeds those of the single CdS and binary noble metal/CdS systems, demonstrating the potential for practical photocatalytic hydrogen production. 相似文献
998.
采用第一性原理电子结构方法研究了四价过渡金属Ti, Zr和Hf替代Cu2ZnSnS4(CZTS)中Sn原子以及Se替代S原子所得到的四元硫族化合物的电子结构、光学性质和晶体结构的稳定性. 实验上用Se替代CZTS中部分S得到的Cu2ZnSnS4-xSex(CZTSSe)作为光吸收材料, 可以进一步提高光伏效率. 我们计算表明用Se替代S后, CZTSe的价带顶明显下移, 并接近Cu(In, Ga) Se2 (CIGS)价带顶位置. 与CZTSe的电子结构特征一样, Cu2Zn(Ti, Zr, Hf)S4四元硫化物的价带顶与母体材料CZTS相比也向低能移动, 并接近CIGS价带顶位置. 由于高光伏效率要求窗口材料ZnO、缓冲层材料和光吸收材料的价带顶和带隙满足一定的渐进的变化关系, 因此可以预见用Cu2Zn(Ti, Zr, Hf)S4作光吸收材料可以有效地提高甚至接近CIGS的光伏效率. 通过计算弹性常数和声子谱, 以及有限温度下第一性原理分子动力学模拟, 发现Cu2Zn(Ti, Zr, Hf)S4的结构稳定性与CZTS相近. 进一步计算Cu2Zn(Ti, Zr, Hf)S4与不同缓冲层间和窗口材料与缓冲层间的反射系数, 并讨论了ZnSe, In2S3, ZnS作为缓冲层材料和TiO2作为窗口材料对光伏效率可能的影响. 相似文献
999.
共沉淀法制备了Ru-Zn催化剂,在ZrO_2作分散剂下考察了助剂前体ZnSO_4浓度对苯选择加氢制环己烯Ru-Zn催化剂性能的影响.并用X-射线衍射(XRD)、X-射线荧光光谱(XRF)、N_2-物理吸附、透射电镜(TEM)和X-射线光电子能谱(XPS)等手段对催化剂进行了表征.结果表明,当ZnSO_4前体浓度低于0.10 mol/L时,Ru-Zn催化剂中Zn以ZnO形式存在,在加氢过程中ZnO可以与反应修饰剂ZnSO_4反应生成(Zn( OH)_2)_3(ZnSO_4)(H_2O)_3盐.继续增加ZnSO_4前体浓度,催化剂中Zn以ZnO和NaZn_4(SO_4)(Cl)(OH)_6·6H_2O盐存在,在加氢过程中ZnO和NaZn_4(SO_4)(Cl)(OH)_6·6H_2O盐可以与反应修饰剂ZnSO_4反应生成(Zn( OH)_2)_3(ZnSO_4)(H_2O)_5.(Zn( OH)_2)_3(ZnSO_4)(H_2O)_x(x=3或5)盐的Zn~(2+)可以转移金属Ru的部分电子.因此,随ZnSO_4前体浓度的增加,(Zn( OH)_2)_3(ZnSO_4)(H_2O)_x的量逐渐增加,金属Ru失电子越多,催化剂活性越低,环己烯选择性越高.0.08 mol/L ZnSO_4前体制备Ru-Zn催化剂给出了59.1%的环己烯收率,而且该催化剂具有良好的重复使用性能和稳定性. 相似文献
1000.
用共沉淀法制备了纳米Ru-Zn催化剂,考察了阿拉伯树胶修饰对苯选择加氢制环己烯催化剂性能的影响,并用X射线衍射(XRD)、透射电镜(TEM)、N_2-物理吸附、X射线光电能谱(XPS)和X射线荧光光谱(XRF)等手段对催化剂进行了表征。结果表明,阿拉伯树胶的用量可以调变Ru-Zn催化剂的粒径。最高环己烯收率随粒径的增大呈火山型变化趋势。当阿拉伯树胶与RuCl_3·x H_2O的质量比为0.033时,Ru-Zn催化剂的最佳粒径为4.0 nm,最高环己烯收率达59.6%。且该催化剂具有良好的重复使用性能。 相似文献