ACS Applied Energy Materials
·
2019
·
IF 0
Hongjie Xu,Minjie Xuan,Weidong Xiao,Yonglong Shen,Zhenzhen Li,Zhuo Wang,Junhua Hu,Guosheng Shao
Solid electrolytes based on theoretically identified double antiperovskite phases Li6OSI2 were successfully synthesized. Experimental characterization supported the theoretical prediction that S substitution of O leads to stabilization of the double antiperovskite structure and lattice softening to significantly enhance ionic conductivity, so that the total Li+ conductivity in Li6.5OS1.5I1.5 was two to three orders better than that of the best stoichiometric antiperovskite phase Li3OCl. However, both antiperovskite and double antiperovskite materials are fundamentally susceptible to surface reconstruction, which is behind significant boundary resistances typically known for materials based on antiperovskite hali-chalcogenides. Such a surface related problem was then effectively reduced through amorphous phase formation, thus offering a feasible route to exploit the full potential of this class of new materials as competitive candidates for solid Li-ion batteries.
研究领域:
材料科学
·
固态电池研究
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产品关联
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jia Hui Guo,Huan Liu,Yong Wang,YaNan Teng,XingWei Sun,Wei Yan Sun,Chun Ping Li,Jie Bai
The development of efficient, stable and low-cost dual-function electrocatalysts and applicated it to Zn-air batteries are very important for the development of renewable energy storage and conversion technologies. Antiperovskite catalysts have attracted much attention recently due to their advantages of adjustable structure and high element selectivity. In this work, a flexible and adjustable antiperovskite catalyst ZnCCe 3−x Ni x (0 ≤ x ≤ 3) loaded on carbon fiber (ZnCCe 3−x Ni x /CNFs) was prepared by electrospinning technology and used as an air cathode catalyst for rechargeable Zn-air batteries. By doping the X-site with highly conductive transition metal Ni, the electronic structure of the catalyst ZnCCe 3−x Ni x /CNFs was optimized, and the catalytic activity of the antiperovskite bimetallic X-site was tuned to achieve an efficient and synergistic catalytic reaction. Among them, ZnCCe 2.7 Ni 0.3 /CNFs showed excellent OER/ORR bi-functional catalytic activity (Δ E = 0.82 V) and good stability. When ZnCCe 2.7 Ni 0.3 /CNFs is used as the cathode catalyst for rechargeable Zn-air batteries, it shows a power density of 117.99 mW cm −2 , and the cycle stability can be maintained for up to 300 h, indicating its application potential in the field of Zn-air batteries.
研究领域:
材料科学
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能源技术
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Shengsheng Fan,Meng Lei,Han Wu,Jiulin Hu,Congling Yin,Tongxiang Liang,Chilin Li
High-conductivity solid electrolytes are crucial components for the development of Na-based solid state batteries . However the electrolyte structure prototype and corresponding synthesis method are still lacking. The conventional oxide and sulfide electrolytes are precursor-expensive (e.g. Na 2 S) or energy-intensive in sintering synthesis (e.g. at 1000 °C). Here, we propose a novel anti-perovskite solid electrolyte of Na-rich fluorinated sulfate (Na 3 SO 4 F) benefiting from Mg and Cl co-doping by solid state reaction from low-cost precursors at moderate temperature (500 °C). The tailored dual doping enables an improvement of ionic conductivity by three orders of magnitude close to 10 −4 S cm −1 at 60 °C. The creation of Na vacancies (by aliovalent Mg doping) and lattice expansion (by substituting F sites with larger-sized Cl ions) are responsible for the conductivity upgrade. A Na–Sn/Fe [Fe(CN) 6 ] 3 solid state battery based on Na 2.98 Mg 0.01 SO 4 F 0.95 Cl 0.05 electrolyte can reversibly run with a first discharge capacity as high as 91.0 mAh g −1 and a reversible capacity preserved at 77.0 mAh g −1 . This result paves a way to novel anti-perovskite family of fluorinated sulfates as potential alkali metal ion solid electrolytes beyond already reported A 3 OX (A = Li or Na, X = heavy halogen or hydrogenide anions) anti-perovskites.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Qian Liang,Yu Zhao,Jian-de Chen,Jia-jun Dai,Xingyu Ding,Zhen Tong,Shi-jun Xie,Jing Zhang,Zhe-hui Zhou,Jun-Tao Li,Jian-Feng Li,Yao Zhou
Anti-perovskites represent a type of newly arising functional materials with a well-defined cubic lattice crystal structure; they provide an excellent entity for studying structure–activity relationship in heterogeneous catalysis. Herein, nitride-based anti-perovskite CuNNi3 was synthesized, and its catalytic properties in electroreduction of carbon dioxide (CO2RR) to syngas were explored for the first time. The introduction of N into the body center of the face-centered cubic cell of CuNi3 was found to create abundant Lewis basic sites with various strengths and thus favored stronger adsorption of the relevant critical species, thus leading to significant improvement in the efficiency of CO2RR and hydrogen reduction compared with that of CuNi3. More importantly, when a thin CuNNi3 nanoshell is coated on a CuNi3 alloy core, significant nanosizing and interfacial interaction effects are noticed, which change the catalytic behaviors of the anti-perovskite. On one hand, the nanosizing effect leads to occurrence of Ni2+ species with a higher oxidative state and consequently deactivates the weak Lewis basic sites in the CuNNi3 nanoshell, which accordingly inhibits hydrogen evolution; the CuNi3@CuNNi3 nanocomposite thus delivers CO Faradaic efficiency up to 96% in comparison to a value of 70% yielded by the bulky counterpart. On the other hand, evident interfacial electron delocalization from the CuNi3 alloy core to the CuNNi3 nanoshell was observed, which was found to increase the N escape energy in the cubic cell of CuNNi3 and consequently enhance its chemical stability; as a result, the CuNi3@CuNNi3 nanocomposite displays much improved catalytic stability compared with the bulky counterpart in CO2RR. This work for the first time explores the interesting electrocatalytic behavior of nitride-based anti-perovskites in electrochemical reduction of CO2, which spells a grand opportunity for the structure–relationship study in CO2RR.
研究领域:
材料科学
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电化学催化
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纳米技术
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DOI
高影响因子
Journal of the American Chemical Society
·
2019
·
IF 14.695
Zhong-Xia Wang,Yi Zhang,Yuan-Yuan Tang,Peng-Fei Li,Ren-Gen Xiong
Antiperovskites have developed to be one kind of important functional material over the past few decades, showing abundant physical properties such as negative thermal expansion and superconductivity, etc. However, antiperovskite ferroelectrics have scarcely been discovered in inorganic ceramics. In this article, we report a new organic–inorganic hybrid antiperovskite ferroelectric [(CH3)2(F-CH2CH2)NH]3(CdCl3)(CdCl4) based on the strategy of molecular design. The replacement of one methyl in [(CH3)3NH]CdCl3 with ethyl produces the lower symmetric [(CH3)2(CH2CH3)NH]CdCl3 with nonpolar perovskite structure, while the polar hexagonal antiperovskite structure with the formula of X3BA (where X = [(CH3)2(F-CH2CH2)NH]+, B = [CdCl3]−, and A = [CdCl4]2–) was received after further fluoridation of the ethyl group. Therefore, fluoridation successfully achieves the structural transformation from perovskite to antiperovskite, as well as the significant changes in physical properties from nonferroelectric to ferroelectric. The antiperovskite [(CH3)2(F-CH2CH2)NH]3(CdCl3)(CdCl4) exhibits typical ferroelectric phase transition above room temperature (Tc = 333 K) including thermal anomalies, dielectric transitions, and second harmonic generation (SHG) responses. Moreover, lower coercive fields and easy polarization switching are observed by the measurements of hysteresis loops and ferroelectric domains. The saturated polarization (Ps) of 4.0 μC/cm2 is almost 10 times as large as those recently discovered antiperovskite molecular ferroelectrics. This finding provides a novel strategy to design and explore more antiperovskite organic–inorganic hybrid ferroelectric materials.
研究领域:
材料科学
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物理学
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DOI
高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 28
·2300695
·
IF 27.8
Zhi Deng,Diancheng Chen,Mingyang Ou,Yuanpeng Zhang,Jia Xu,Dixing Ni,Zhaoran Ji,Jiantao Han,Yang Sun,Shuai Li,Chuying Ouyang,Zhaoxiang Wang
Recently, a new family of anti-perovskite Li 2 TMSO was discovered as promising cathode materials for Li-ion batteries (LIBs) with superiorities in high specific capacity, low cost, and environmental friendliness. However, the applications of these anti-perovskite materials meet severe challenges in the cyclability and rate performance. Herein, a cation-disordered anti-perovskite type solid solution Li 2 Fe 1− x Mn x SO (LFMSO, x = 0, 0.2, 0.5) with excellent electrochemical performance is reported. On the basis of comprehensive structural characterizations, the role of the cation disordering in LFMSO is clarified. In comparison with Li 2 FeSO (LFSO), the reduced Li-ion diffusion barrier and the increased Li-rich octahedral configurations in LFMSO with higher configurational entropy imply the facilitated long-range Li-ion diffusion and the suppressed phase transition, which favor the high-rate capability and cycling stability. In addition, the large lattice distortion and Coulombic interaction between the anions and cations lead to the breathing of the unit cell during charge/discharge. The variation of the unit cell volume decreases to 2.5% upon Li-ion delithiation. A superstructure is observed in LFMSO for the first time. These findings help to pave the way for the research and development of novel cathode materials for the next generation LIBs.
研究领域:
材料科学
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电化学
·
固态化学
·
能源存储
·
锂电池
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DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 40
·21265-21272
·
IF 11.301
Lei Gao,Hao Zhang,Yuechao Wang,Shuai Li,Ruo Zhao,Yonggang Wang,Song Gao,Lunhua He,Hai-Feng Song,Ruqiang Zou,Yusheng Zhao
Sodium-rich antiperovskite (NaRAP) ionic conductors have been considered promising inorganic electrolytes for all-solid-state sodium batteries due to their low fabrication cost, high sodium ionic conductivity and good structural tolerance. The high structural flexibility of NaRAPs allows variety of chemical substitutions to improve conductivity; in particular, the substitution of the anion cluster has effectively proved promoting Na+ migration, both experimentally and theoretically. Herein, we report an unexpected boost in Na+ ionic conductivity that climbs to 0.37 mS cm−1 at 485 K by introducing NO2− groups in the antiperovskite Na3ONO2 system. Its mechanism was fully investigated by neutron powder diffraction and DFT calculations, proving that the NO2− group on the lattice center, can utilize its terminal O2− anion to facilitate the Na+ migration via the Na–O interaction, when thermally excited at 485 K. The detailed migration path is also discussed by both maximum entropy method (MEM) and DFT calculations.
研究领域:
材料科学
·
固态离子学
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无机化学
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能源材料
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计算材料学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Haitao Wang,Juan He,Lei Ge,Zhi Xu,Wei Zhou,Zongping Shao
Although many metal-based compounds demonstrate the ability to detect glucose, limited metal compounds have the desired high conductivity. Metal nitrides with different states of metal elements (M), such as M 0 and M 2+/3+ , can perform excellent conductivity and catalytic activity. In this work, self-supported non-enzymatic electrochemical sensors supported by carbon paper (CP) were synthesized for monitoring glucose in alkaline solutions. The antiperovskites FeNNi 2 Co and FeNNi 3 as electrocatalysts are first reported in the field of the electrochemical sensor, displaying outstanding catalytic activity and high electrical conductivity. Electrochemical tests suggest that the FeNNi 2 Co/CP and FeNNi 3 /CP electrodes perform outstanding sensing abilities toward rapid glucose determination. In addition, the FeNNi 2 Co with multi-metals can display the trimetallic synergic effect and superior performance than the original material of FeNNi 3 . The sensitivity of FeNNi 2 Co/CP electrode can reach level of 3621 and 1141 μA mM −1 cm −2 in the concentration ranges of 2–2789 μM and 2789–7444 μM, respectively. The repeatability of the glucose concentration in the glucose drink measured by the FeNNi 2 Co/CP electrode can achieve 96.2%.
研究领域:
材料科学
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电化学
·
传感器
·
分析化学
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产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2025
·
IF 8.9
Weigao Zhong,Qiming Sun,Jinsong Wang,Xiang Ao,Yuling Zhai,Tao Zhu,Xing Zhu,Hua Wang,Zhishan Li,Kongzhai Li,Chundong Wang
Owing to the structural and compositional flexibility feature, antiperovskites have garnered widespread attention, and been regarded as promising catalysts. However, their intrinsic sluggish kinetics impede their practical applications. Herein, a CoN 0.73 Co 3 @CoFeN(OH) x is constructed by a developed oxidation technology, endowing exceptional performance toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at ampere-level current densities. The advanced nature of our as-prepared antiperovskite could be further evidenced by an assembled alkaline electrolyzer (CoN 0.73 Co 3 @CoFeN(OH) x ||CoN 0.73 Co 3 @CoFeN(OH) x ), yielding a current density of 1000 mA/cm 2 with 1.89 V, and stable working for over 100 h. Operando characterizations clarify that iron atoms in the antiperovskite skin promote the generation of CoOOH active species. Theoretical calculations are referred to understand the decent catalytic activity, which reveals that Fe atoms are responsible for the favorable adsorption of the OOH oxygen intermediate and modulate the hydrogen adsorption strength. This work paves a solid way for engineering the antiperovskites for green hydrogen generation applications.
研究领域:
材料科学
·
电化学
·
催化
·
能量转换
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jia-Hui Guo,Huan Liu,Yu-Xuan Gao,Xiao-Peng Liu,Jie Bai
The key to the commercial available of Zinc Air batteries (ZABs) is to design and exploit the low-cost and high efficiency bifunctional oxygen electrocatalysts. Here, it is reported that a bifunctional electrocatalyst consisting of nitrogen-rich carbon nanotubes encapsulating antiperovskite ZnCNi 3 nanoparticles grafted onto the surface of carbon nanofibers (ZnCNi 3 -NCCF) for rechargeable ZABs. The electrocatalytic activity of ZnCNi 3 -NCCF is promoted by the synergistic catalysis of graphitic nitrogen-doped carbon and antiperovskite ZnCNi 3 . The ZnCNi 3 -NCCF (1,3,3–9 h) with moderate graphitic nitrogen-doped carbon species exhibits low overpotentials (half-wave potential ( E 1/2 ) = 0.75 V vs. RHE for oxygen reduction reaction (ORR), the potential to achieve current density of 10 mA cm −2 ( η 10 ) = 352 mV for oxygen evolution reaction (OER)) and Favourable stability. It was showed that graphitic-N-C in ZnCNi 3 -NCCF enhances OOH ⁎ adsorption to optimize activity of ORR by the Density functional theory (DFT) calculations. Additionally, the ZnCNi 3 -NCCF-based ZABs stable charge-discharge cycling for 200 h and light up a 4 V light-emitting diode (LED) bulb for 12 h, thereby showcasing certain practical application prospects
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产品关联
DOI
PubMed
高影响因子
Frontiers in Chemistry
·
2021
·
IF 5.221
Yu Pengcheng,Ye Yu,Zhu Jinlong,Xia Wei,Zhao Yusheng
Solid-state lithium metal batteries have attracted broad interest as a promising energy storage technology because of the high energy density and enhanced safety that are highly desired in the markets of consumer electronics and electric vehicles. However, there are still many challenges before the practical application of the new battery. One of the major challenges is the poor interface between lithium metal electrodes and solid electrolytes, which eventually lead to the exceptionally high internal resistance of the cells and limited output. The interface issue arises largely due to the poor contact between solid and solid, and the mechanical/electrochemical instability of the interface. In this work, an in situ “welding” strategy is developed to address the interfacial issue in solid-state batteries. Microliter-level of liquid electrolyte is transformed into an organic–inorganic composite buffer layer, offering a flexible and stable interface and promoting enhanced electrochemical performance. Symmetric lithium–metal batteries with the new interface demonstrate good cycling performance for 400 h and withstand the current density of 0.4 mA cm−2. Full batteries developed with lithium–metal anode and LiFePO4 cathode also demonstrate significantly improved cycling endurance and capacity retention.
研究领域:
材料科学
·
电化学
·
储能技术
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电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Photonics
·
2024
·
IF 32.3
Liu Lang,Liu Shi-Yu,Shi Yuanpeng,Fang Cui-Ling,Zhao Shan,Shen Huai-Yi,Chen Ming-Xing,Wang Ze-Jie,Ma Yan,Liu Yan,Feng Yan,Tang Jiang,Ye Heng-Yun,Niu Guangda
Halide perovskites have shown promising potential for direct X-ray detection due to their high X-ray absorption coefficient, low trap states and convenient fabrication process. However, it is still a challenge to achieve high sensitivity, low dark current and low detection limit in a single material. The deep reason for this is the trade-off between the material’s μτ product and resistivity. Here we report the construction of an organic–inorganic hybrid anti-perovskite ((2-Habch) 3 Cl(PtI 6 )) with indirect transition and low orbital symmetry at the band edge to achieve an ultralong intrinsic lifetime and thus break the trade-off. (2-Habch) 3 Cl(PtI 6 ) achieves an unprecedented long carrier lifetime of >3 ms, leading to a large μτ product of 6.25 × 10 −3 cm 2 V −1 and high resistivity of 10 12 Ω cm, outperforming most X-ray detection materials. These properties enabled the development of X-ray detectors that simultaneously achieve an ultralow dark current of 0.21 nA cm −2 , high sensitivity of 1.0 × 10 4 µC Gy air −1 cm −2 , ultralow detection limit of 2.4 nGy air s −1 and excellent operational stability with no observable baseline drift, outperforming state-of-the-art perovskite single-crystal detectors. The rare combination of high performance in almost every figure of merit in the anti-perovskite-based X-ray detector could enable new-generation X-ray detection systems.
研究领域:
材料科学
·
物理学
·
放射学
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产品关联
DOI
高影响因子
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