Inorganics
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2023
·Vol. 11
·期 6
·243
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IF 2.9
Xiantun Huang,Chenglin Lu,Yun Li,Haimei Tang,Xingqing Duan,Kuikui Wang,Haizhen Liu
MgH2has a high hydrogen content of 7.6 wt% and possesses good reversibility under normal conditions. However, pristine MgH2requires a high temperature above 300 °C to release hydrogen, with very slow kinetics. In this work, we utilized Ti3CN MXene to reduce the operating temperature and enhance the kinetics of MgH2. The initial temperature of MgH2decomposition can be lowered from 322 °C for pristine MgH2to 214 °C through the employment of Ti3CN. The desorbed MgH2+ 7.5 wt% Ti3CN can start absorption at room temperature, while the desorbed pristine MgH2can only start absorption at 120 °C. The employment of Ti3CN can significantly improve the hydrogen release kinetics of MgH2, with the desorption activation energy decreasing from 121 to 80 kJ mol−1. Regarding thermodynamics, the desorption enthalpy changes of MgH2and MgH2+ 7.5 wt% Ti3CN were 79.3 and 78.8 kJ mol−1, respectively. This indicates that the employment of Ti3CN does not alter the thermal stability of MgH2. Phase evolution studies through the use of X-ray diffraction and electron diffraction both confirm that Ti3CN remains stable during the hydrogen release and uptake process of the composite. This work will help understand the impact of a transition metal carbonitride on the hydrogen storage of MgH2.
研究领域:
材料科学
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能源存储
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Chunli Wang,Na Yang,Dongxue Cai,Shu-Zhong Zhan,Kun Liu
The electrocatalytic processes of hydrogen evolution reaction and hydrogen oxidation reactions have emerged as global strategies to address critical environmental and energy challenges associated with fossil fuel consumption. To enhance electrocatalytic activity, we focus on the design of novel electrocatalysts based on first-row transition metal complexes. A new nickel complex [Ni(dppe)Cl 2 ] by the reaction of NiCl 2 with 1,2-bis(diphenylphosphino)ethane (dppe) were synthesized and characterized in our group. The structure of nickel complex was determined cryptographically. The electro-catalyze hydrogen evolution (HER) activity of complex Ni(dppe)Cl 2 in acetonitrile solution with acetic acid as proton and a neutral buffer (pH 7.0) medium was evaluated by controlled potential electrolysis, with a turnover frequency (TOF) of 155 and 366 (mol of H 2 /mol of cat/h), respectively. Notably, electrocatalytic activity towards hydrogen oxidation (HOR) in acetonitrile solvent using Ni(dppe)Cl 2 as a catalyst has also been studied, and the complex exhibits highly catalytic efficiency with a TOF of 0.77 s −1 . The above results indicate that the Ni complex can be act as promising electrocatalyst for HER and HOR.
研究领域:
化学
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材料科学
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能源研究
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Man Chen,Yiqi Wang,Xuezhang Xiao,Yunhao Lu,Meng Zhang,Jiaguang Zheng,Lixin Chen
Magnesium hydride (MgH 2 ) has attracted extensive attention over the past decades due to its highly reversible hydrogen storage density (7.6 wt%). But intrinsic high activation energy barriers for de/rehydrogenation of MgH 2 /Mg restrict its potential application as an on-board hydrogen carrier. Herein, ZrH 2 nanocatalyst homogeneously distributed on the surfaces of MgH 2 exhibits pronounced low temperature de/rehydrogenation kinetics, resulting from the vast lattice distortions between ZrH 2 and MgH 2 /Mg phases. The ZrH 2 doped MgH 2 composite (MgH 2 -ZrH 2 ) starts to release H 2 at 203 °C, 102 °C lower than that of undoped MgH 2 . Most importantly, MgH 2 -ZrH 2 quickly absorbs 5.90 wt% H 2 at the temperature as low as 65 °C. Further deep investigations found that H atoms preferentially accumulates around ZrH 2 , since the lower hydrogen dissociation energy on the surfaces of ZrH 2 (1.421 eV) than that of pure Mg (2.301 eV). Then, the large lattice disordered zone between ZrH 2 and Mg phases enables H atoms diffuse easily into the lattice of Mg nearby, thus triggering the formation of MgH 2 . These findings are critically important to understand the mechanism of other metal hydride catalysts, as well as offer an opportunity for the practical on-board fuel cell applications in the future.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
ACS Catalysis
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2019
·
IF 12.221
Xueping Qin,Lulu Zhang,Gui-Liang Xu,Shangqian Zhu,Qi Wang,Meng Gu,Xiaoyi Zhang,Chengjun Sun,Perla B. Balbuena,Khalil Amine,Minhua Shao
Improving the reaction kinetics of hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is critical to promote the development of alkaline fuel cells and electrolyzers. Here, we prepared Pd3Ru alloy nanocatalysts with Ru segregated on the surfaces, forming adatoms and clusters. This structure dramatically lowered the overpotential of Pd toward HER in 1 M KOH by 104 mV at 10 mA cm–2. The HER activity was even higher than that of Pt (6 mV improvement at 10 mA cm–2). Theoretical simulation results revealed that Ru adatoms/clusters on the surface could weaken the hydrogen-binding energy and promote the OH adsorption, consequently lowering the reaction barrier of the rate-determining step in HER. Our findings are of significance for clarifying the role of Ru in bimetallic catalysts and rational design of more active catalysts for HER/HOR.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yuzhi Li,Janel Abbott,Yanchun Sun,Jianmin Sun,Yunchen Du,Xijiang Han,Gang Wu,Ping Xu
Here, in an effort to prepare Ru-based metal organic frameworks, we developed a one-step solvothermal synthesis for Ru nanoassembly catalysts, which consist of ˜4 nm Ru nanoparticles well dispersed on amorphous carbon (Ru/C). The Ru/C catalyst obtained from a mixed solvent of H 2 O and CH 3 CH 2 OH (Ru/C-H 2 O/CH 3 CH 2 OH), featured a chain-like porous structure, provides Pt-like catalytic properties with low overpotentials at −10 mA cm −2 for the hydrogen evolution reaction (HER) within a wide range of pH values, i.e., 35 mV in 0.5 M H 2 SO 4 , 53 mV in 1.0 M KOH, and 93 mV in 3.5 wt% NaCl. Ru/C is also an efficient hydrogen oxidation reaction (HOR) catalyst at all pH values. In the alkaline media, Ru/C-H 2 O/CH 3 CH 2 OH achieves a mass activity of 41.1 mA mg -1 at an overpotential of 50 mV and a high exchange current density (0.65 mA cm −2 ). The work provides a facile strategy to synthesize highly active Ru/C catalysts for bifunctional HER and HOR electrocatalysis.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhentong Wang,Zhiqiang Gong,Yusan Turap,Yidi Wang,Zhe Zhang,Wei Wang
An integrated recycling waste bioenergy and manufacturing low-carbon hydrogen by a method to convert biogas to hydrogen based on the chemical looping concepts was proposed in this study. Biogas from biomass anaerobic digestion and pyrolysis was employed in the reduction step as the feedstock of fuel gas. Simulated marsh gas (CH 4 and CO 2 ) and pyrolysis gas (CO and H 2 ) were used to validate the feasibility of the reduction performance with iron (III) oxide at different reaction temperatures. The experiments were conducted by using a thermogravimetric analyzer and a tandem packed-bed reactor. As for marsh gas, the reaction behavior was completely different under different CO 2 concentrations and converting temperatures. The reduction reaction with CH 4 would be divided into three stages, including complete combustion, competition reaction, and partial oxidation stage. Furthermore, the syngas with a tailored ratio of 1:1 can be produced without CH 4 breakthrough by adjusting CO 2 concentration. Besides, the total H 2 production achieved 241.9 mL per gram of oxygen carrier with a purity of 98.29%. Regarding the pyrolysis gas, the solid conversion and CO breakthrough curve were investigated. Compared to a single reactor, seven reactors were required to increase the average solid conversion from 34.1% to 42% and reduced the total redox time from 705.6 min to 437.7 min. Overall, this study provided a link between waste bioenergy recycling and H 2 generation with a novel chemical looping hydrogen generation (CLHG) system and supplied theoretical support for scaling up the packed-bed reactor to improve H 2 production efficiency.
研究领域:
能源生物学
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环境工程
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Wanli Liang,Mengyan Zhou,Xiulan Li,Lijie Zhu,Zhixin Li,Yifan Zhou,Jian Chen,Fangyan Xie,Hao-Fan Wang,Nan Wang,Yanshuo Jin,Hui Meng
Hydrogen energy is the most suitable solution for long-term, large-scale energy storage, and the design of efficient, economical, and stable electrocatalysts for hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) is of great significance for its commercial development. Herein, Ni nanocluster supported on oxygen-vacancy-rich MoO 2 (Ni/MoO 2−x ) is designed which contains a large number of oxygen vacancies and Ni–O–Mo bonds. According to X-ray photoelectron spectroscopy, the formation of oxygen vacancies and Ni–O–Mo bonds facilitates the transfer of electrons from Ni to O. The prepared Ni/MoO 2−x @NF shows excellent hydrogen electrocatalytic activity, which is proved by a Tafel slope of only 26 mV dec −1 for HER and an exchange current density of 3.64 mA cm −2 for HOR. Theoretical calculations showed optimized free energy of hydrogen adsorption and hydroxide adsorption on Ni/MoO 2−x , which can explain the origin of the high activity of the catalyst. This work provides a feasible strategy for designing non-precious metal hydrogen electrocatalytic materials in energy storage.
研究领域:
材料科学
·
能源存储与转换
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DOI
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Xue Gao,Long Hu,Yuchen Mao,Zeming Zhong,Liangjun Huang,Kaisheng Xia,Hui Wang,Min Zhu
Porous carbon materials (PCMs) hold great promise as hydrogen storage materials due to their high capacity but are limited by adsorbing H2 at either cryogenic temperature or very high H2 pressure due to their weak van der Waals forces with the H2 molecules. In this study, N-doped hierarchical porous carbon (NHPC) materials were prepared by a simple one-step chemical activation method. Experimental results reveal that N-doping significantly enhances the interaction between H2 and the PCMs, which is demonstrated by increased adsorption isosteric heat (Qst) and H2 storage capacity per specific surface area (SSA). At lower H2 coverage, the Qst increases from 7.45 kJ/mol (NHPC-0) to 7.95 kJ/mol (NHPC-2 and NHPC-3), which aligns with the enhanced gravimetric H2 uptake per SSA. At higher H2 coverage (77 K, 50 bar-H2), there is a notable enhancement in the volumetric H2 uptake per SSA for NHPC-3 (11.41 g·L–1/m2·g–1) compared to that for NHPC-0 (8.49 g·L–1/m2·g–1) as the N content increases. Furthermore, N-doping can increase the packing density, thereby improving the volumetric H2 storage capacity of NHPC-x. The enhancement is strikingly demonstrated by NHPC-2, which achieves a volumetric H2 uptake of 26.96 g/L (SSA = 2458.44 m2/g) at 77 K and 50 bar. This is almost the same as that for NHPC-0, despite a 21% reduction in SSA, which is 26.47 g/L (SSA = 3116.58 m2/g) at the same condition. This work contributes to a deeper understanding of the effect of heteroatom doping on the H2 storage performance in PCMs.
研究领域:
材料科学
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化学工程
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能源存储
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongjie Yu,Shaojian Jiang,Wenjie Zhan,Yuqin Liang,Kai Deng,Ziqiang Wang,You Xu,Hongjing Wang,Liang Wang
The high cost is a major issue that has contributed to the slow industrialization of electrolytic water. To reduce the cell voltage to below 0.5 V, we constructed a hybrid electrolytic water system with coupled hydrogen evolution reaction (HER) and formaldehyde oxidation reaction (FOR). For FOR, the abundant Cu 0 and Cu + in nitrogen-doped Cu/Cu 2+1 O on Cu foam (N-Cu/Cu 2+1 O/CF) can effectively promote the adsorption and activation of H 2 O and HCHO molecules, and facilitate the cleavage of O-H and C-H, while nitrogen doping can promote the exposure of Cu active sites. For HER//FOR, a cell voltage of only 0.42 V is required to achieve 500 mA cm −2 . The system can not only produce H 2 routinely at the cathode through HER but also release H 2 by HCHO oxidation. The construction of a dual hydrogen production system with industrial current density at ultra-low voltage provides a new idea to reduce the cost of hydrogen production.
研究领域:
能源科学
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电化学
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材料科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Youpeng Cao,Hongling Liu,Yuxuan Xiao,Lun Li,Jiao Yang,Chunfa Liu,Chengcheng Zhong,Wendi Zhang,Shuyang Peng,Junge Yang,Zhichao Yu,Weng Fai Ip,Hui Pan
Platinum (Pt) is a highly efficient catalyst for the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR). However, the scarcity of Pt necessitates the development of catalysts with low Pt content while maintaining high activity. In this study, we report the synthesis of oxygen-modified supra-nanometer-sized RuPt nanocrystals with low Pt content by a simple air annealing method to achieve a catalyst with high activity. The annealed catalyst, RuPt/C-200, exhibits a very low overpotential of only 3.8 mV at 10 mA cm−2, a low Tafel slope of 16.6 mV dec−1, and a 2.8-fold increase in mass activity at an overpotential of 0.06 V for HER compared to the unannealed catalyst. Additionally, the HOR exchange current density increases 2.9-fold compared to the unannealed catalyst. AEMWE tests confirm the application potential of RuPt/C-200, while density-functional-theory (DFT) calculations reveal that oxygen modification, by optimizing the hydrogen binding energy, plays a crucial role in improving the catalytic performance of RuPt. This work highlights that combining the oxygen modification strategy with the nanoscale size effect could advance the development of high-performance RuPt electrocatalyst for both alkaline HER and HOR.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Mengyuan Jin,Xiang Han,Ting Chou,Shuangyan Li,Yecan Pi,Kai Chen,Tingting Chen,Shun Wang,Yun Yang,Juan Wang,Huile Jin
Developing highly efficient electrocatalyst with heterostructure for hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is crucial to the fabrication and conversion of hydrogen energy but also remains a great challenge. Herein, the synthesis of ruthenium-nickel nanoparticles (Ru 3 -Ni NPs) with heterostructure for hydrogen electrocatalysis is reported, and studies show that their catalytic activity is improved by electron redistribution caused by the distinctly heterogeneous interface. Impressively, Ru 3 -Ni NPs possess the remarkable exchange current density (2.22 mA cm −2 ) for HOR. Additionally, an ultra-low overpotential of 28 mV is required to attain a current density of 10 mA cm −2 and superior stability of 200 h for HER. The highly efficient catalytic activity can be attributed to the electron transfer from Ni to Ru and the optimal adsorption of H* on Ru-Ni sites. Our study showcases a reliable heterostructure that boosts the HOR/HER activity of the catalyst in alkaline environments. This work provides a new pathway for designing high-performance electrocatalyst for energy storage and conversion.
研究领域:
材料科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
·
2021
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IF 2.328
Dongxin He,Wei Cao,Deshun Huang,Haimin Li,Jing Zhu,Pengxiang Zhao
Safety use of hydrogen leads to the development of highly sensitive materials for hydrogen sensing. Herein, Pd(II)@alkyne-PVA/ d -Ti 3 C 2 T x composite was prepared by spin-coating Pd(II)@alkyne-PVA solution onto the filter membrane supported with delaminated Ti 3 C 2 T x ( d -Ti 3 C 2 T x ). The properties of the composite were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, and X-ray photoelectron spectroscopy (XPS). The results demonstrate that the composite shows high sensitivity and stability for hydrogen sensing.
研究领域:
材料科学
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化学工程
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纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）