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INORGANIC CHEMISTRY · 2024 · IF 4.3

Mechanochemical Synthesis of High-Entropy MOF-74 with Multiple Active Sites for CO2 Adsorption and Synergistic Conversion

Liang Ye,Ya Zhang,Siyang Jin,Chaohui Zhou,Junbao Pang,Yunjie Luo,Yuhang Yu,Wei Xu

Compared with monometallic metal–organic frameworks (MOFs), the synergistic effect of multiple metals significantly enhances the catalytic performance of the CO2 cycloesterification reaction, leading to improved CO2 adsorption and catalytic conversion capabilities. To investigate this concept, a high-entropy MOF-74 (HE-MOF-74) with a uniform distribution of five distinct metal ions (Zn2+, Mg2+, Ni2+, Co2+, and Cu2+) was successfully synthesized using a straightforward mechanical ball milling technique and comprehensively characterized (including structural, morphological, and physicochemical properties). The results reveal that HE-MOF-74 exhibits significantly increased specific surface area and CO2 adsorption capacity compared with those of monometallic MOF-74. The presence of multiple unsaturated metal centers as Lewis acid sites, oxygen atoms linking the metals, and ligand-based hydroxyl groups serving as base sites enable efficient immobilization of CO2 into cyclic carbonate. This study introduces a novel synthetic approach for the green and efficient production of HE-MOF-74 and proposes a new application for CO2 utilization.

研究领域: 材料科学 · 环境科学 · 催化化学
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ACS Applied Energy Materials · 2020 · IF 4.473

Millimeter Silicon-Derived Secondary Submicron Materials as High-Initial Coulombic Efficiency Anode for Lithium-Ion Batteries

Lijing Yan,Huiwen Zhang,Zeheng Li,Xuehui Gao,Hongbo Wang,Zhan Lin,Min Ling,Chengdu Liang

Nanostructured silicon has been regarded as a promising next-generation anode material for high energy density lithium-ion batteries. However, costly synthesis methods and low initial coulombic efficiency are still two major challenges for its practical application. Herein, secondary submicron silicon materials composed of nanoparticles are successfully prepared by a simple, low-cost, and efficient high energy mechanical milling method. The initial coulombic efficiency of the as-prepared silicon anode reaches 89.14% with a first discharge specific capacity of 3233 mA h g–1 at 100 mA g–1. In light of a low-cost precursor, facile approach, and high initial coulombic efficiency, this work may provide guidance and enlightenment in synthesizing nanostructured silicon with a secondary structure as anode materials for lithium-ion batteries.

CAS / MDL: 7440-21-3
研究领域: 材料科学 · 能源存储
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Energetic Materials Frontiers · 2022 · IF 0

Catalytic properties of CuO–Cr2O3–PbO ternary nanocomposites favorable for the pyrolysis of ammonium perchlorate

Guang-pu Zhang,Yu-hang Cheng,Miao-miao Li,Lei Xiao,Hu Guo,Wei Jiang,Ga-zi Hao

In this study, CuO–Cr 2 O 3 –PbO ternary nanocomposites (TNCs) with different atomic ratios of Cu:Cr:Pb (5:2:8, 5:4:6, 5:6:4, 5:8:2) were synthesized by means of efficient mechanical milling. As confirmed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM), uniform and impurity-free CuO–Cr 2 O 3 –PbO TNCs with an average grain size of 30 ​nm were successfully obtained. The catalytic properties of CuO–Cr 2 O 3 –PbO TNCs favorable for the pyrolysis of ammonium perchlorate (AP) were studied through thermogravimetric (TG) analysis and differential scanning calorimetry (DSC). The results show that TNC-8, which has an atomic ratio of 5:8:2 (Cu:Cr:Pb), exhibited the highest catalytic activity for the pyrolysis of AP when the pyrolytic temperature of AP decreased from 441.3 ​°C to 360.2 ​°C and the Gibbs free energy ( Δ G ≠ ΔG≠ ) decreased from 199.8 ​kJ·​mol −1 to 175.2 ​kJ·​mol −1 , as compared to CuO–Cr 2 O 3 –PbO nanocomposites with other atomic ratios.

研究领域: 材料科学 · 催化化学
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RARE METALS · 2024 ·Vol. 43 ·期 5 ·1999-2014 · IF 9.6

Graphdiyne (CnH2n-2) as an “electron transfer bridge” boosting photocatalytic hydrogen evolution over Zn0.5Co0.5S/MoS2 S-scheme heterojunction

Li Mei,Wang Jing-Zhi,Jin Zhi-Liang

In the process of photocatalytic water cracking, the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the catalyst. In this paper, a carbon isotope superconducting material graphdiyne (GDY) is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn 0.5 Co 0.5 S/MoS 2 inorganic system. In terms of hydrogen evolution kinetics, GDY acts as an electron bridge, not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated charges. Morphologically, the large two-dimensional layer provides more loading and anchoring points for Zn 0.5 Co 0.5 S/MoS 2 , which increases the number of active sites. The ternary composite catalyst 20%GDY/Zn 0.5 Co 0.5 S/Mo 2 S (20-GCSM) generates 69.94 μmol of hydrogen (5 h) in triethanolamine solution. It is 2.97 and 1.80 times higher than Zn 0.5 Co 0.5 S and Zn 0.5 Co 0.5 S/MoS 2 , respectively. After the cyclic experiment, it still has stable hydrogen evolution performance after standing for 24 h (under dark conditions). In addition, the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron spectroscopy. This work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges. Graphical abstract

研究领域: 材料科学 · 催化 · 纳米技术 · 能量转换 · 固体物理
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Energy Technology · 2020 ·Vol. 8 ·期 10 ·2000606 · IF 3.404

Low-Cost Raw Materials Synthesized Na2.9375PS3.9375Cl0.0625 Solid Electrolyte

Yu Wang,Nachuan Yang,Yi Shuai,Kanghua Chen

Na 3 PS 4 -based materials, which have relatively high conductivities, make promising Na-ion solid electrolytes for realizing all-solid-state sodium batteries. Herein, Na 2.9375 PS 3.9375 Cl 0.0625 solid electrolytes’ power is prepared by a mechanical ball milling process and subsequent heat treatment process using low-cost Na, NaCl, P 2 S 5 , and S as raw materials. In addition, its electrical conductivity and electrochemical performance by compounding with polyethylene oxide–NaClO 4 are studied. The results show that Na 2.9375 PS 3.9375 Cl 0.0625 solid electrolyte heated at 550 °C with polyethylene oxide–NaClO 4 exhibits Na-ion conductivity of 8.75 × 10 −4 S cm −1 . The pragmatic and cost-effective raw materials grant the solid electrolyte with high-performance and higher practical value.

研究领域: 材料科学 · 电化学 · 能源存储 · 固体离子学 · 无机非金属材料
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SOLID STATE IONICS · 2016 · IF 2.38

High-temperature performance of all-solid-state battery assembled with 95(0.7Li2S-0.3P2S5)-5Li3PO4 glass electrolyte

Shanshan Mo,Penghao Lu,Fei Ding,Zhibin Xu,Jiaquan Liu,Xingjiang Liu,Qiang Xu

Sulfide glasses with a high lithium-ion conductivity are promising solid electrolyte for all-solid-state lithium-ion batteries. In this study, 95(0.7Li 2 S–0.3P 2 S 5 )–5Li 3 PO 4 glass electrolyte is prepared by mixing 70Li 2 S-30P 2 S 5 (mol%) glass and Li 3 PO 4 crystal using mechanical milling technique. The effects on the structures and electrochemical properties of the obtained ternary sulfide glass were examined. The ternary sulfide glass shows a good electrochemical stability, which may exhibit a wide electrochemical window up to 10   V (vs. Li/Li + ). Furthermore, the 95(0.7Li 2 S-0.3P 2 S 5 )-5Li 3 PO 4 glass electrolyte displays an electrical conductivity of 2.513   ×   10 −   3   S   cm −   1 at 100   °C. The all-solid-state lithium-ion cell assembled with 95(0.7Li 2 S-0.3P 2 S 5 )-5Li 3 PO 4 glass electrolyte shows a favourable cyclability, which can reveal a discharge capacity of 144   mAh   g −   1 at 0.05   °C and a discharge capacity of 63.9   mAh   g −   1 at 0.1C after the 50th cycle at 100   °C, respectively.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 锂电池技术
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 34 ·16273-16279 · IF 3.925

Lead-free broadband orange-emitting zero-dimensional Sb3+-doped indium-based organic–inorganic metal halides

Haiming Cheng,Chi Cao,Ying Zhang,Dayang Wang,Wensheng Yang,Renguo Xie

Low-dimensional organic–inorganic metal halides have shown great application potential and new opportunities for use in solid-state lighting due to their excellent optical and electronic properties. However, the most studied hybrid compounds contain lead, which limits their application environments. The preparation of organic–inorganic metal halides with high luminous efficiency, long-term stability, and a lead-free composition for environmental protection has become an important goal for the design of materials. Here, novel Sb3+-doped indium-based metal halides, (CH3NH3)4InCl6·Cl, have been designed and synthesized via a simple mechanical ball milling method; in the lead-free zero-dimensional (0D) halide (CH3NH3)4InCl6·Cl, isolated [InCl6]3− octahedra are separated by methylamine cations. Under UV excitation, the bulk-phase powder exhibits broadband orange-yellow emission peaking at 607 nm with a full width at half-maximum of ∼160 nm upon incorporating Sb3+ into the (CH3NH3)4InCl6·Cl matrix. The photoluminescence quantum yield (PLQY) of Sb3+-doped (CH3NH3)4InCl6·Cl is as high as 67.72%. The effects of the Sb3+-doping concentration on the crystal structure and optical characteristic have been investigated. The indirect band gap characteristics of (CH3NH3)4InCl6·Cl were demonstrated via density functional theory (DFT) calculations, and the relatively wide band gaps of 3.83 eV and 2.99 eV of (CH3NH3)4InCl6·Cl and (CH3NH3)4ClInCl6:Sb3+ were experimentally determined. These experimental results suggest that the as-prepared Sb3+-doped (CH3NH3)4InCl6·Cl has potential applications in solid-state lighting devices.

研究领域: 材料科学 · 无机化学 · 光电子学 · 固体照明 · 半导体材料
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