APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Bowen Lu,Tai Zhang,Liqi Zhang,Yongqing Xu,Zewu Zhang,Fan Wu,Xiaoshan Li,Cong Luo
CeO 2 -based catalysts have been widely used in the CO 2 hydrogenation process. The oxygen vacancies on CeO 2 resulted from Na ion incorporation play a vital role in CO 2 conversion activity, the effect of Na + ion-doped in CeO 2 during CO 2 hydrogenation was rarely studied. In this work, the LN-CeO 2 catalysts with different n NaOH :n Ce ratios were prepared with liquid nitrogen(Liquid Nitrogen-CeO 2 , LN-CeO 2 ), and the effect of the n NaOH :n Ce ratio on the microstructure of the LN-CeO 2 catalysts were evaluated. The best CO 2 hydrogenation performance was achieved by LN-CeO 2 -100 with a CO production rate of 3.90 mol/g cat· h at 800 °C (100% CO selectivity). The kinetic results indicated that the CO 2 hydrogenation performance difference among these LN-CeO 2 catalysts resulted from the CO 2 activation process. Oxygen vacancies could enhance CO 2 activation on the surface of LN-CeO 2 , and oxygen vacancies displayed a linear correlation relationship with the Na content doped in LN-CeO 2 . The highest concentration of oxygen vacancies resulted from Na ion incorporated and lower CO 2 reaction order was closely related to CO 2 hydrogenation performance of LN-CeO 2 -100. These results will give insight into the Na effect on the CO 2 hydrogenation mechanism over CeO 2 .
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 39
·15067-15073
·
IF 4.569
Yi Huang,Junben Huang,Yong Zhang
Metal thiophosphates have aroused much research interest due to their structural chemistry and possible applications as infrared functional materials. In this study, five quaternary Sr-based alkali metal thiophosphates ASrPS4 (A = Li, Na, K, Rb, Cs) were obtained. Their structural comparison shows that their symmetry undergoes transformation from tetragonal (I41/acd) to monoclinic (P21/c) to orthorhombic (Pnma) system, which is induced by the cation size effects and coordination features of different alkali metal cations. The experimental and theoretical results demonstrate that the band gaps of all title compounds are large, namely 3.6–3.9 eV (experimental results) and 3.78–4.12 eV (HSE06). Theoretical analyses indicate that the [PS4] group could be regarded as a good unit for designing wide band gap compounds, and the birefringence of NaSrPS4 is 0.08 at the fundemental 1064 nm wavelength, which shows that it may be a potential infrared birefringent material.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jianhui Zhu,Linchao Zeng,Xiaoya Li,Ning Zhao,Yanyi Wang,Zhilan Lin,Tingshu He,Libo Deng,Peixin Zhang
The inexpensive room-temperature sodium-sulfur (RT Na-S) battery has attracted extensive attention due to its various potential application but is still suffering from the low utilization of sulfur, the shuttle effect and the sluggish reaction activity of sodium polysulfides (SPSs). In this work, a TiO 2 /sulfur/atomic-iron loaded carbon nanosheet cathode is designed for high performance RT Na-S battery. When the atomic iron exists, a much higher electrochemical activity of sulfur was obtained, indicating the atomic iron can accelerate the conversion of SPSs. Furthermore, the TiO 2 layer can inhibit the shuttle effect of SPSs and the side-reaction between the intermediates and carbonate electrolyte. As a result, the constructed sulfur cathode exhibits a high reversible capacity (569.9 mAh g −1 with an initial coulombic efficiency of 57.57%) at 0.1 A g −1 and outstanding cycling performance (507 mAh g −1 after 50 cycles). This work provides a new strategy for preparing high performance cathode materials for RT Na-S battery.
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Advanced Energy Materials
·
2022
·Vol. 12
·期 37
·2201734
·
IF 29.698
Qi Li,Jun Zhang,Lixiang Zhong,Fushan Geng,Ying Tao,Chuannan Geng,Shuzhou Li,Bingwen Hu,Quan-Hong Yang
Hard carbons have been identified as competitive anodes for Li/Na/K-ion batteries but their Li/Na/K-ion storage mechanisms significantly vary in different batteries. It is fundamental to understand the basic science behind the difference. Herein, it is theoretically revealed that defects on the carbon layers generally have an influential impact on the atomic interactions including the metal–metal (M–M) and metal–carbon (M–C) interactions, thereby determining whether the stored alkali-metal atoms are in ionic or quasi-metallic states. Upon increasing the number of metal atoms on a carbon layer composed of only hexatomic rings, K tends to be stored in an ionic state similar to Li due to the dominant M–C interaction, while on a carbon layer with defects, K tends to be stored in a quasi-metallic state similar to Na due to the dominant M–M interaction. For experimental verification, a glassy carbon, the extreme form of hard carbon with dominant sp 2 hybridization and only Stone–Wales defects, is selected as a model anode, and its Li/Na/K-ion storage mechanisms are exactly consistent with the theoretical prediction. More profoundly, for the first time, the quasi-metallic K cluster information is captured by ex situ electron paramagnetic resonance.
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SOLAR ENERGY
·
2022
·
IF 7.188
Wenhu Zhang,Pin Lv,Yujiao Li,Yangqing Wu,Jia Dong,Wenzhi Wang,Hairui Sun,Bingqiang Cao
Hole transport layer free perovskite solar cells (HTL-Free PSCs) have attracted extensive attention due to their advantages of simple structure and low cost. However, due to the serious energy level mismatch caused by the direct contact between the perovskite layer and the opposite electrode, the space for improving the efficiency of HTL-Free PSCs is greatly limited. We use Eu 3+ doped CsPbBr 3 quantum dots (QD) to modify the interface between MAPbI 3 :Na layer and C electrode, and study its effect on the surface defect passivation, interface energy level arrangement and carrier transport behavior in the device. It was found that compared with the interfacial modification of CsPbBr 3 QD alone, the interfacial modification of CsPbBr 3 :Eu QD could effectively solve the problem of energy level mismatch in HTL-Free PSCs, resulting in a remarkable improvement of conversion efficiency from 9.01 % to 12.95 %. Furthermore, electron beam induced current (EBIC) was used to prove that CsPbBr 3 :Eu QD interface modification significantly improved the hole collection ability. This provides an experimental basis and theoretical guidance for the optimization of the efficiency of other types of transport layer free photovoltaic devices.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2021
·Vol. 105
·期 2
·1300-1317
·
IF 3.784
Yan Xie,Xue Geng,Yuan Wang,Jiang Guo,Yuhui Lu,Qiuyi Lv,Zhijiang Ma,Dan zhang,Jin Zhao,Bin Deng,Ruijin Yu
High-efficiency and far-red light phosphors based on Mn 4+ -doped inorganic luminescence materials are beneficial to plant cultivation. However, Mn 4+ -doped oxide phosphors have a common problem of low quantum efficiency. Alkali metal ion codoping can effectively improve the luminescence properties of Mn 4+ -activated oxide phosphors. Herein, a series of Sr 2 InSbO 6 :Mn 4+ , M (SISO:Mn 4+ , M) (M = Li + , Na + , and K + ) far-red-emitting phosphors codoped alkali metal ions were first synthesized. Density functional theory calculation indicated that SISO is a kind of indirect bandgap material with a bandgap of ∼1.60 eV. The SISO:Mn 4+ samples showed a far-red light at 698 nm upon 365 nm, which perfectly matched the absorption spectrum of the far-red-phytochrome (Pfr) of plants. The doping concentration of the SISO:Mn 4+ samples was optimized to be 0.006 mol. The concentration quenching mechanism was defined as dipole–dipole interaction by combining the Dexter theory and the Inokuti–Hirayama model. Optimizing the sintering temperature and codoped with alkali metal ions (Li + , Na + , and K + ) could improve the luminescent intensity of SISO:Mn 4+ . The optimum sintering temperature was 1300°C. The internal quantum efficiencies of SISO:0.006Mn 4+ and SISO:0.006Mn 4+ , 0.006Li + phosphors are 22.67% and 60.56%, respectively. SISO:Mn 4+ , Li + phosphors-based plant growth light-emitting diodes (LEDs) demonstrate excellent optical stability and long lifetime. Thus, these phosphors are promising candidates for plant cultivation LEDs.
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Small
·
2021
·Vol. 17
·期 40
·2101650
·
IF 13.281
Zhengying Wang,Yue Xu,Jian Peng,Mingyang Ou,Peng Wei,Chun Fang,Qing Li,Jiang Huang,Jiantao Han,Yunhui Huang
Taking into the consideration safety, environmental impact, and economic issue, the construction of aqueous batteries based on aqueous electrolyte has become an indispensable technical option for large-scale electrical energy storage. The narrow electrochemical window is the main problem of conventional aqueous electrolyte. Here, an economical room-temperature inorganic hydrated molten salt (RTMS) electrolyte with a large electrochemical stability window of 3.1 V is proposed. Compared with organic fluorinated molten salts, RTMS is composed of lithium nitrate hydrate and sodium nitrate with much lower cost. Based on the RTMS electrolyte, a hybrid Li/Na-ion full battery is fabricated from cobalt hexacyanoferrate cathode (NaCoHCF) and perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) anode. The full cell with the RTMS electrolyte exhibits a fantastic performance with high capacity of 139 mAh g −1 at 1 C, 90 mAh g −1 at 20 C, and capacity retention of 94.7% over 500 cycles at 3 C. The excellent performances are contributed to the unique properties of RTMS with a large electrochemical window, solvated H 2 O free and high mobility of Li + , which exhibits excellent Li-ions insertion and extraction capacity of NaCoHCF. This RTMS cell provides a new economic choice for large-scale energy storage.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Qimeng Peng,Ju Fu,Gang Chen,Dong Feng,Tianbiao Zeng
Antimony sulfides exhibit a tremendous potential owing to the high theoretical specific capacity from multiple redox storage mechanisms for sodium-ion batteries (SIBs). However, these bottlenecks, including low electrical conductivity , poor ionic diffusion kinetics, and severe volume expansion, still restrict the development of antimony sulfide as SIBs anodes. Meanwhile, in view of long-term interests and practical application, the cost-efficient preparation methods become an imminent challenge to the advancement of high-performance SIBs anodes. Here, a novel three-step strategy, composed of co-precipitation, heat reduction processes, and sulfation conversion, was utilized to construct a “reinforced concrete” architecture, in which Sb 2 S 3 nanoparticles embedded in N-doped carbon matrix (NC) modified by carbon nanotubes (CNTs), denoted as Sb 2 S 3 /CNTs/NC. As the “cement block”, the N-doped 3D carbon matrix can promote the electron migration and reduce the aggregation of active materials upon cycling. In terms of “rebars” (i.e., 1D CNTs) for ensuring the anode integrality during incessant sodiation/de-sodiation processes, they function as binders and stabilizers , which intimately cross-link with Sb 2 S 3 nanoparticles and carbon matrix, accommodate the volume change, and maintain the fast transfer of electron transfer inside the whole composite. Benefiting from these merits of the hierarchical structure (i.e., 3D NC and 1D CNTs), as an anode for SIBs, Sb 2 S 3 /CNTs/NC demonstrates an improved sodium storage capability with an initial specific capacity of 770.80 mAh g −1 at 0.1 A g −1 and a superior initial coulombic efficiency (ICE) of 79.90%. Moreover, even at a high current density of 1.0 A g −1 , a reversible capacity of 313.54 mAh g −1 can be delivered after 350 long cycles, indicating the stable cyclicity. The Sb 2 S 3 /CNTs/NC with designed construction and enhanced electrochemical performance could provide a new perspective on low-cost, time-saving, and exercisable synthesis approach for high-performance sulfide-based anodes.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Jingyu Xu,Yangyang Xie,Jingqiang Zheng,Congyin Liu,Yanqing Lai,Zhian Zhang
Sodium (Na) metal anode has been considered as the promising candidate for next generation high-energy-density rechargeable batteries such as Na-S, Na-O 2 and Na-CO 2 , owing to its high specific capacity, low electrode potential and low cost. Unfortunately, some intractable problems hinder the practical application, including volume change and dendrite formation induced by inhomogeneous Na nucleation. Herein, 3D carbon cloth (CC) supporting Bi-MOF derived carbon nanosheets containing Bi nanoparticles and carbon shells (CC@Bi@C) were prepared to serve as Na deposition/dissolution hosts, integrating high surface area and favorable sodiophilicity. Due to the existence of Bi sodiophilic sites, Na nucleation and deposition can be induced, rendering uniform and dendrite-free morphology. Moreover, the 3D carbon framework can effectively reduce the current density and uniform distribution of Na + flux, solving the uncontrolled Na dendrite growth. As a result, the CC@Bi@C||Na half cell operating at 1 mA cm −2 for 1 mA h cm −2 exhibits 99.85% Coulombic efficiency for nearly 500 cycles. The symmetric cell maintains stable cycle for more than 300 h at 2 mA cm −2 for 2 mA h cm −2 with low overpotential. When paired a full cell with Na 3 V 2 (PO 4 ) 3 cathode, CC@Bi@C anode exhibits a stable capacity of 103.4 mA h g −1 at 1C (1 C = 117 mA h g −1 ) over 150 cycles for 95.5% capacity retention with high CE of 99.0%. This work provides a facile strategy to inhibit dendrite growth and uniform Na deposition.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Tianbiao Zeng,Dong Feng,Qimeng Peng,Qi Liu,Guocui Xi,Gang Chen
Among the germanium-based compounds, GeTe is a promising anode candidate that exhibits high theoretical capacity (856 mAh g–1 vs Li+/Li and 401 mAh g–1 vs Na+/Na) and low volume expansion during an ion intercalation/deintercalation process. Nevertheless, achieving good dispersion of metal-like GeTe in anode materials remains a significant challenge. Herein, hybrid GeTe/graphene (GeTe/G) is proposed as a highly efficient anode for LiBs and SiBs by facile ball milling. Pulverized GeTe is effectively anchored on peeled graphene sheets that can accelerate Li+ transport in electrodes as predicted by theoretical calculations and thus result in improved overall electrochemical performance. For instance, GeTe/G possesses a high reversible capacity of 478 mAh g–1 under 0.1 A g–1 in the 300th cycle. Moreover, by further cross-linking the GeTe/G using carbon nanotube (CNT) and carbon nanofiber pyrolysis from cotton cellulose, the as-prepared three-dimensional (3D) flexible anode possesses macropores that acted as positive channels favorably for ion transport. Remarkably, the as-prepared flexible 3D GeTe/G/CNT electrode with a thickness of 1050 μm exhibits a high reversible capacity of 451.4 mAh g–1 (4.38 mAh cm–2) vs Li+/Li and 372.5 mAh g-1 (2.08 mAh cm-2) vs Na+/Na, respectively, in the second cycle under 0.1 A g–1. These results shed some light on the direct application of 3D flexible carbon sponge electrodes in high-performance LiBs/SiBs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Weifeng Tu,Chao Sun,Zhengzhou Zhang,Wenqi Liu,Haripal Singh Malhi,Wei Ma,Minghui Zhu,Yi-Fan Han
This work unravels the chemical and structural properties of Fe 5 C 2 -ZnO catalysts decorated with sodium (Na) during CO 2 hydrogenation to linear α-olefins, determined by rate assessments and series of in-situ characterizations. Reaction network remains as a combination of reverse water-gas-shift (RWGS) and CO hydrogenation, but their relative contributions vary. The RWGS reaction is chemically equilibrated, thus CO 2 conversion is determined solely by the thermodynamic constraint. However, Na addition alleviates the formation rates of paraffins from the subsequent CO hydrogenation and reactions of olefins with hydrogen. Na additive does not alter the structures of Fe 5 C 2 -ZnO, but improves largely the stability of Fe 5 C 2 by preventing the phase oxidation during the reaction. Na modifies the surface properties of catalyst, thus facilitates reaction of CO* and H* and the C C bond formation. The dual role of Na leads more effective olefins turnovers and provides new insights to the design of novel catalysts for CO 2 utilization.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2021
·
IF 2.694
Kuo Zhou,Xingfan Wang,Junfang Yang,Fenli Jin,Huan Zhou
The solubility equilibrium of Li+, Na+//Cl–, CO32– −H2O quaternary systems at 323.15 K and 348.15 K was studied via the isothermal solubility equilibrium method, and the complete phase diagrams were obtained including the properties of liquid density and pH. Solid species of LiCl·H2O, Li2CO3, NaCl, and Na2CO3·H2O are found in the quaternary system at 323.15 K and 348.15 K, and one double salt of Li2CO3·Na2CO3 is found at 348.15 K. The liquid phase of two invariant points and five univariant curves at 323.15 and three invariant points and seven univariant curves at 348.15 K in the quaternary system is determined. Li2CO3 covers the largest solid phase region and is hardly influenced by temperature; Li2CO3–NaCl is a stable salt pair, and its cosaturated solubility is the least at the diagonal line of Li2CO3–NaCl.
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