CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Yichen Qi,Zeyang Zhang,Qinke Tang,Jiangchuan Liu,Rui Shi,Jiguang Zhang,Yana Liu,Jun Wang,Jiankun Zhang,Shihao Chen,Yunfeng Zhu
Catalysis has been demonstrated to be effective in enhancing the kinetics of MgH2, which has been widely investigated as one of the most promising solid-state hydrogen storage materials. It is essential and challenging to design catalysts with high activity and to understand the corresponding interaction mechanisms between the catalysts and MgH2, especially for multiphase catalyst systems. In this study, an elaborated VS2/NiS2 catalyst based on well-combined components and heterostructure is exploited to substantially improve the hydrogen storage performance of MgH2. Impressively, rapid dehydrogenation (3.4 wt % H2 in 900 s at 498 K) and low-temperature hydrogenation (3.7 wt % H2 in 7200 s at 348 K) properties are achieved in the MgH2–VS2/NiS2 system. The activation energies for the hydrogen absorption/desorption are calculated to be 32.1/86.7 kJ mol–1, which represents a considerable reduction of 60.9% and 43.6% compared to the as-milled MgH2, respectively. Detailed investigations reveal that the enhanced hydrogen absorption/desorption kinetics are mainly attributed to the synergistic effect induced by the in situ-formed Mg2Ni/VH2 heterostructure and the “hydrogen pump” of Mg2Ni/Mg2NiH4. The Mg2Ni/VH2 heterostructure elongate Mg–H bonds, while the “hydrogen pump” of Mg2Ni/Mg2NiH4 facilitate H transfer. This work offers a fresh perspective for application of multicomponent catalysts in the field of metal hydrides.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yuge Yan,Xiaofeng Gu,Mingyang Zhou,Zhijie Wang,Xifen Gong,Yu Chen,Qingyu Li,Jiang Liu
Here we use the electrochemical hydrogen pump derived from a protonic ceramic cell (PCC) to realize the first demonstration of separating hydrogen from simulated peanut shell pyrolysis gas (64% H 2 , 26% CO, 4% CO 2 , and 6% CH 4 ). The single PCC is configured with a thick Ni–BaCe 0.7 Zr 0·1 Y 0·2 O 3-δ cathode, a thin BaCe 0·7 Zr 0·1 Y 0·18 Fe 0·02 O 3-δ electrolyte, and an Ag–Ce 0.8 Gd 0.2 O 1.9 anode with an effective area of 1.5 cm 2 . At 650 °C and a feeding current density of −500 mA cm −2 , a hydrogen flux of 2.34 ml min −1 cm −2 , a Faradaic efficiency of 62%, and a hydrogen recovery rate of 29% are achieved. In addition, 20 wt% Ni is mixed into the Ag-GDC electrode to achieve a hydrogen flux of 3.68 ml min −1 cm −2 and a Faradaic efficiency of 97%. Additionally, a 20-h measurement for PCCs with the Ni-mixed electrode shows the hydrogen fluxes and Faradaic efficiencies of above 1.49 ml min −1 cm −2 and 98%, respectively.
研究领域:
能源科学
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材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 24
·14629-14637
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IF 10.733
Chong Lu,Yanling Ma,Fan Li,Hong Zhu,Xiaoqin Zeng,Wenjiang Ding,Tao Deng,Jianbo Wu,Jianxin Zou
A core–shell nanostructured Mg@Pt composite, consisting many of icosahedral Mg particles as the core with nano-sized Pt particles distributed homogeneously on different surfaces, was synthesized through an arc plasma method followed by the generic solid-state method. The microstructures and hydrogen sorption properties of the Mg@Pt composite were carefully investigated and compared to that of pure Mg powder. In particular, the dehydrogenation behaviors of the hydrogenated Mg@Pt composite were observed in situ via high-resolution transmission electron microscopy (HRTEM). The results revealed that the Pt on Mg particles showed a “spillover” effect to improve the hydrogen absorption kinetics in the early stage. It then transformed into H-stabilized Mg3Pt, followed by the formation of MgH2. DFT calculation and in situ TEM observations demonstrated that the H-stabilized Mg3Pt acted as a “hydrogen pump” for the dehydrogenation of MgH2 and then transformed into Pt after desorption. Through this effect, the dehydriding kinetics of the hydrogenated Mg@Pt composite was improved and the onset dehydrogenation temperature was reduced compared to that of the pure MgH2 powder.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Fang Liu,Jiali Wang,Wei Chen,Xiaoying Zhang,Shengting Li,Jinping Li,Yu-Fei Song,Jinfeng Chu,Guang Liu
Magnesium hydride (MgH 2 ) is broadly deemed as one of the most prospective solid-state hydrogen storage materials. However, its large-scale application is hindered by several drawbacks, including an excessive dehydrogenation temperature (>300 °C), sluggish kinetic behavior, and inevitable agglomeration and growth during cycling. To address these challenges, two-dimensional few-layered laminated titanium carbide catalyst (FL-Ti 3 C 2 T x ) was synthesized via LiF/HCl etching followed by liquid-phase ultrasonic exfoliation. These FL-Ti 3 C 2 T x nanosheets exhibit efficient catalytic activity for MgH 2 hydrogen storage. The incorporation of 5 wt% FL-Ti 3 C 2 T x significantly reduces the initial dehydrogenation temperature of MgH 2 from 325 °C to 199 °C, while enabling the dehydrogenated sample to reabsorb hydrogen at room temperature. The MgH 2 + 5 wt% FL-Ti 3 C 2 T x composite demonstrates remarkable kinetic performance, releasing 6.5 wt% H 2 within 8 min at 300 °C and uptaking 5.49 wt% H 2 within 1 min at 100 °C. Even after 50 cycles of consecutive dehydrogenation and rehydrogenation, the composite retained a hydrogen storage capacity of 6.90 wt%, corresponding to a 95.30 % capacity retention rate. Microstructure analysis and theoretical calculations reveal that the unique lamellar morphology of FL-Ti 3 C 2 T x not only provides abundant active sites and hydrogen diffusion paths, but also effectively suppresses the agglomeration and growth of Mg/MgH 2 matrix during the hydrogen absorption and desorption. More importantly, the in-situ formed Ti/TiH 2 functions as a “hydrogen pump” accelerating hydrogen diffusion, prolonging the Mg H bond length, and weakening the interaction between Mg and H. These factors synergistically enhance the absorption/desorption kinetics of MgH 2 .
研究领域:
储能
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材料科学
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纳米技术
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氢能
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Sanyang Guo,Zhichao Yu,Yuan Li,Yaokun Fu,Zhuohan Zhang,Shumin Han
Magnesium hydride (MgH 2 ) is a promising hydrogen storage material with high weight and volume hydrogen capacity. However, higher operating temperature and reversible hydrogen capacity decay inhibit its wide application. To address these issues, Mg-Mg 2 Ni/C was obtained by ball milling magnesium and nickel-Metal Organic Framework (Ni-MOF), and following calcinations . Initial dehydrogenation temperature of the composite is 530 K, 70 K lower than that of MgH 2 , and the apparent activation energy of the composite is 77.6 ± 2.1 kJ/mol, which is only 50% of MgH 2 . At 423 K, the hydrogen capacity of the composite is about 6 wt% within 3600 s, and keeps unchanged after ten cycles. The carbon material introduced by Ni-MOF inhibits the agglomeration of Mg, and Mg 2 Ni/Mg 2 NiH 4 acts as a “hydrogen pump” in de/hydrogenation process. The carbon coating and “hydrogen pump” lead to the improvement of the ab/desorption kinetics and cycling stability. This attempt paves a potential way to achieve high performance Mg-based composite hydrogen storage materials.
研究领域:
材料科学
·
储氢技术
·
能源材料
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yiyang Zeng,Shuai Yang,Mao Yang,Yu Gong,Xingrui Tang,Xiaolong Fu,Junyan Wang,Guangming Ran,Chengjian Xiao
Hydrogen separation and purification play a crucial role in the chemical industry. High-temperature electrochemical hydrogen pump (HT-EHP) technology based on polybenzimidazole (PBI) membranes has great potential for hydrogen purification, the key to this application lies in the design of PBI membranes with high proton conductivity. To achieve this, we optimized the spatial conformation of polymer chains by coordinating metal ions (Zn 2+ /Co 2+ ) with the imidazole groups in PBI, forming continuous coordination cavities. Molecular dynamics (MD) simulations revealed that the coordination between metal ions and imidazole induces polymer chain distortion, creating sub-nanometer coordination cavities (∼8 Å). Wide-angle X-ray scattering (WAXS) and wide-angle X-ray diffraction (WAXD) confirmed the existence of these coordination cavities. After the removal of metal ions, the residual cavities were filled with phosphoric acid (PA), constructing long-range ordered proton conduction pathways in the high-performance PBI membranes ( o -PBI-Zn and o -PBI-Co). Scanning electron microscopy (SEM) analysis showed that the continuous porous network within the polymer chains resembles a root-like structure, facilitating efficient three-dimensional proton transport. The resulting membranes exhibited excellent mechanical properties (tensile strength of 45 MPa) and outstanding proton conductivity (0.126 S/cm at 160 °C). When assembled into a HT-EHP, the membranes achieved a hydrogen purification rate of 9.22 mL (cm 2 ·min) −1 at 180 °C, with an energy consumption as low as 0.1 kWh/L(H 2 ). This study presents an innovative strategy for designing high-proton-conductivity PBI membranes, significantly enhancing their potential for HT-EHP applications, offering a promising alternative for hydrogen purification technologies.
研究领域:
材料科学
·
化学工程
·
膜技术
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能源技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Wen Liao,Fangxia Xie,Lulu Zhang,Qing Xi,Long Cao,Yawen Wang,Yunfang Wang,Houfen Li,Rui Li,Caimei Fan,Jianxin Liu,Jiancheng Wang
Photocatalytic water splitting for hydrogen evolution (PHE) is an effective and sustainable strategy to alleviate energy shortages and environmental issues. However, active hydrogen (H*), as a critical intermediate, has low generation and desorption rates that limit the development of PHE. Herein, a ZnCdS/MoO 3-x heterojunction is prepared by a two-step solvothermal method and applied to a photocatalytic hydrogen evolution reaction under visible light conditions. The band structure and electron spin resonance (ESR) confirm the formation of an S-scheme heterojunction in ZnCdS/MoO 3-x , promoting the utilization of photo-generated carriers and thereby enhancing H* generation on ZnCdS. Furthermore, in-situ ESR, quasi in-situ Raman spectroscopy and in-situ DRFTIRS spectroscopy demonstrate that the H* is subsequently transferred from ZnCdS to MoO 3-x via the hydrogen spillover effect. The H* is then confined within the lattice of MoO 3-x and forms H x MoO 3-x in situ. Finally, the electrochemical tests and DFT calculations demonstrate that the H x MoO 3-x acts as a “hydrogen pump”, lowering the H* desorption barriers and ultimately enhancing the hydrogen evolution of the system. Therefore, the optimum hydrogen evolution rate of ZnCdS/MoO 3-x reaches 7.9 mmol·g −1 ·h −1 , which is 26.3 times higher than that of pure ZnCdS, along with a hydrogen storage capacity of 0.36 wt%. This work offers a novel approach for achieving efficient and sustained PHE reactions by modulating the generation and desorption rates of the intermediate H*.
研究领域:
光催化
·
材料科学
·
能量转换
·
环境科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）