Inorganics
·
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
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Muhammad Asim,Alibek Kurbanov,Bushra Maryam,Muhammad Ajmal,Chenxiang Shi,Lun Pan,Ji-Jun Zou
Incorporating g-C 3 N 4 with transition metal phosphides is emerging as a low-cost and robust co-catalyst for hydrogen evolution . The ammonia borane hydrolysis is an efficient method to release H 2 at ambient conditions in the presence of a catalyst. An efficient and cheap catalyst is needed for practical application to achieve this benchmark. For this purpose, a catalyst Ni 2 P/C 3 N 4 is synthesized by hydrothermal method and low-temperature phosphidation. The optimization reveals that the Ni 2 P/C 3 N 4 with 6.5% Ni contents shows the best performance for H 2 release. Furthermore, 2% Pt nanoparticles loading over Ni 2 P/C 3 N 4 boosts the charge transfer and improves activity 5.7-fold compared to Ni 2 P/C 3 N 4 , and the Pt-loaded catalyst is depicted as Pt@Ni 2 P/C 3 N 4 . The reaction kinetics reveals that the hydrogen evolution rate accelerates by increasing the amount of Pt@Ni 2 P/C 3 N 4 and AB concentration, and the loading of Pt nanoparticles loaded over Ni 2 P/C 3 N 4 reduces the activation energy significantly. Moreover, the ionic interaction between Pt and Ni 2 P/C 3 N 4 generates Ptᵟ + and (Ni 2 P/C 3 N 4 )ᵟ − active sites which facilitates B–H cleavage and O–H bonds of ammonia borane and water, respectively. Incorporating transition metals phosphide and noble metals supported over g-C 3 N 4 paves the pathway toward the efficient H 2 evolution from ammonia borane, bringing cost-effective modifications to synthesize constructive catalysts.
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
·
2020
·
IF 4.939
Senliang Xi,Xiaojun Wang,Kudzaishe Caren Tome,Tonghuan Zhang,Zongying Han,Meng Gao,Shixue Zhou,Hao Yu
In this work, NaBH 4 +2MgH 2 doped by ZrF 4 was prepared by the ball-milling method. The structure and the morphology of different systems were characterized by X-ray diffraction and scanning electron microscopy. The thermodynamic properties of hydrogen release were determined by temperature-programmed desorption and differential scanning calorimetry . Hydrogen desorption kinetic properties and hydrogen content were investigated by pressure composition isothermal method. The main objective of this work was to study the relationship between the heat of hydrogen release and the quantity of hydrogen released by In-situ calorimetry measurement. The NaBH 4 +2MgH 2 +0.1ZrF 4 can release about 7.4 wt.% H 2 by two steps. Firstly, the heat of hydrogen release of the first and the second steps were lower by 480.82 J·g −1 and 430.8 J·g −1 than that of NaBH 4 +2MgH 2 , respectively. And the dehydrogenation enthalpy of NaBH 4 +2MgH 2 went from −243.81 kJ·mol −1 to −191.2 kJ·mol −1 . Secondly, the addition of ZrF 4 can improve the hydrogen release kinetic property of NaBH 4 +2MgH 2 , which can release 5 wt.% H 2 in 2.5 h at 385 °C under 0.01 MPa hydrogen pressure. Therefore, NaBH 4 +2MgH 2 +0.1ZrF 4 will be a potential candidate as a fuel cell hydrogen supply system.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Yugang Shu,Jiaguang Zheng,Chengguo Yan,Ao Xia,Meiling Lv,Zhenxuan Ma,Zhendong Yao
NaBH 4 was widely regarded as a low-cost hydrogen storage material due to its high-mass hydrogen capacity of approximately 10.8% (mass) and high volumetric hydrogen capacity of around 115 g·L –1 . However, it exhibits strong stability and requires temperatures above 500 °C for hydrogen release in practical applications. In this study, two polyhydric alcohols, xylitol and erythritol (XE), were prepared as a binary eutectic sugar alcohol through a grinding-melting method. This binary eutectic sugar alcohol was used as a proton-hydrogen carrier to destabilize NaBH 4 . The 19NaBH 4 -16XE composite material prepared by ball milling could start releasing hydrogen at 57.5 °C, and the total hydrogen release can reach over 88.8% (4.45% (mass)) of the theoretical capacity. When the 19NaBH 4 -16XE composite was pressed into solid blocks, the volumetric hydrogen capacity of the block-shaped composite could reach 67.2 g·L –1 . By controlling the temperature, the hydrogen desorption capacity of the NaBH 4 -XE composite material was controllable, which has great potential for achieving solid-state hydrogen production from NaBH 4 .
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Xuelei Feng,Jianguang Yuan,Yujie Lv,Bogu Liu,Haixiang Huang,Bao Zhang,Youhua Yan,Shumin Han,Ying Wu
Magnesium borohydride (Mg(BH 4 ) 2 ) is an attractive materials for solid-state hydrogen storage due to its high hydrogen content (14.9 wt%). In the present work, the dehydrogenation performance of Mg(BH 4 ) 2 by adding different amounts (10, 20, 40, 60 wt%) of two-dimensional layered Ti 3 C 2 MXene is studied. The Mg(BH 4 ) 2 -40 wt% Ti 3 C 2 composite releases 7.5 wt% hydrogen at 260 °C, whereas the pristine Mg(BH 4 ) 2 only releases 2.9 wt% hydrogen under identical conditions, and the onset desorption temperature decreases from 210 °C to a relative lower temperature of 82 °C. The special layered structure of Ti 3 C 2 MXene and fluorine plays an important role in dehydrogenation process especially at temperatures below 200 °C. The main dehydrogenation reaction is divided into two steps, and activation energy of the Mg(BH 4 ) 2 -40 wt% Ti 3 C 2 composite is 151.3 kJ mol −1 and 178.0 kJ mol −1 , respectively, which is much lower than that of pure Mg(BH 4 ) 2 .
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kun Liu,Yinshi Li
Formic acid (FA), a liquid hydrogen storage carrier, can release hydrogen via photothermal catalysis, providing a clean and sustainable solution toward a carbon-neutral energy cycle. Despite recent advances in the design of efficient catalysts, the development of advanced systems with high H2 yield, stability, and durability remains challenging due to the inefficient photothermal conversion and mass transfer in the traditional liquid–solid bulk system, as well as the trade-off between hydrogen storage density and dehydrogenation rate. Here, we address these challenges by creating a photothermal-induced dual-interface characterized by high spectral absorption and low heat loss, a facile supply of FA, and vaporization of FA to minimize the energy barrier of the reaction. As a result, a record hydrogen evolution rate (200.9 mmol g–1 h–1) is achieved in a high concentration (26 M) of FA, which is about 15 times higher than the liquid–solid bulk system. In addition, it can be operated continuously for more than 192 h without additive addition and energy consumption, providing a strategy for accelerating interfacial mass transfer to improve catalytic activity, and also presents a reference for sustainable hydrogen production.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
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
·
能源科学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2019
·
IF 4.309
Zhencan Hu,Haiying Qin,Xuezhang Xiao,Man Chen,Meijia Liu,Ruicheng Jiang,Lixin Chen
NaMgH3 has been considered to be a potential candidate for solid-state hydrogen storage due to its considerable hydrogen gravimetric (6.0 wt %) and volumetric (88.0 g/L) densities. Meanwhile, NaMgH3 possesses an outstanding theoretical thermal storage density of 2881 kJ/kg, which makes it one of the most promising thermal energy storage materials. However, the sluggish dehydrogenation kinetics of NaMgH3 embarrasses further practical application. Doping a nanosize Ti-based catalyst is treated to be one of the most effective methods to settle the poor dehydriding kinetics. In this work, different kinds of TiO2 catalysts, the 5 wt % TiO2 microparticle (MP) (100 nm), TiO2 nanoparticle (NP) (5–10 nm), and TiO2 nanotube (NT) (5–10 nm), were doped into NaMgH3 in the process of ball milling and heat treatment, which in situ formed Na0.46TiO2 significantly promoting the full hydrogen desorption kinetics of NaMgH3. Among all samples, the TiO2 NT-doped sample shows the best performance of which the onset decomposition temperature is reduced to 300 °C, and the first- and second-step decomposition peak temperatures are decreased to 346.3 and 355.8 °C, respectively. The TiO2 NT-doped sample desorbs approximately 3.4 wt % H2 at 350 °C within 10 min, while the pure NaMgH3 sample releases only 0.2 wt % H2 in 10 min. The significant improvement in both two decomposition reactions kinetics of NaMgH3 can be attributed to the tubular morphology of the TiO2 NT and the in situ formation of multivalence Ti species (Na0.46TiO2). These two reasons can change the kinetic models of NaMgH3 from A2 to R2 and further dramatically decrease the activation energies of first- and second-step decomposition reactions of NaMgH3 to 91.7 and 142.1 kJ/mol, respectively. In particular, the in situ formed Na0.46TiO2 can benefit the e– transfers among Na+, Mg2+, and H–, tremendously enhancing dehydrogenation properties.
研究领域:
材料科学
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能源工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Kang Chen,Mili Liu,Liuzhang Ouyang,Hui Wang,Jiangwen Liu,Min Zhu
Hydrolysis of LiBH 4 (LB in short) is considered as a potential means of releasing the hydrogen stored in the hydride and the water. However, the hydrolysis of LB occurs only above 0 °C and efficient catalysts are required to accelerate the hydrogen kinetics. Here, we demonstrate an efficient non-catalytical hydrogen generation system that enables H 2 production of LB over a wide range of temperatures with methanol (referred to MeOH), ethylene glycol, and MeOH/water mixtures as reaction solvents. The results indicate that the hydrogen kinetics of LB is controllable by MeOH dose, MeOH species, reaction temperature, and solution components. For instance, the hydrogen evolution rate could be accelerated from 266 to 515 mL H2 min −1 g −1 (per unit weight of LB) with a H 2 yield up to 93% by tailoring the dose of methanol at 25 °C. Notably, the glycolysis kinetics is much faster than that for the methanolysis of LB, delivering a hydrogen rate varying from 523 to 10,125 mL H2 min −1 g −1 . By optimizing reaction conditions, a gravimetric hydrogen density of ~4.6 wt% H 2 was realized in the LB-MeOH system. Interestingly, the methanolysis/glycolysis products of LB can spontaneously convert into MeOH and hydrated byproduct (LiBO 2 ‧2H 2 O) by reacting with water, and MeOH may be separated and reused as an intermediate. Here, LiBO 2 ‧2H 2 O can be easily regenerated back to LB by ball milling with Mg under ambient conditions. Thus, a hydrogen cycle combining hydrogen generation and storage in a closed material cycle is achieved, which may lay the foundation for developing practical hydrogen sources for mobile/portable applications.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xiang Gong,Shuyi Guo,Zhao Jiang,Bolun Yang,Tao Fang
Hydrogen is a promising candidate to substitute the fossil fuels. However, the efficient hydrogen storage technologies restrict the commercial applications. Developing new catalysts with high activity and selectivity is important for the dehydrogenation reaction in N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NECZ/12H-NECZ) hydrogen storage system. In this work, a series of Pd-M/Al 2 O 3 (M = Co, Ni and Cu) bimetallic catalysts are synthesized successfully and show good performance in the dehydrogenation reaction of 12H-NECZ than the commercial Pd/Al 2 O 3 catalyst. The Pd 1 Co 1 /Al 2 O 3 catalyst (Practical Pd content = 2.4136 wt%) showed the highest catalytic performance with 95.34% H 2 release amount, TOF of 230.5 min −1 and 85.4% selectivity of NECZ. Combined with the characterization analysis, it can be proposed that the dehydrogenation performance of 12H-NECZ is dependent on the alloy phases , reasonable electronic structures and nanoparticle size of catalysts. The fine-tuned alloy degree and appropriate nanoparticle size of Pd 1 Co 1 /Al 2 O 3 bring the 17.7% increase of H 2 release amount and 99.5% increase of NECZ selectivity than those of Pd/Al 2 O 3 . For the bimetallic catalysts, the enhancement of selectivity of NECZ is mainly from the increase of the kinetic constant of rate-limiting step.
研究领域:
催化化学
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材料科学
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能源存储
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Shigang Li,Xiaohui Liu,Yong Guo,Yanqin Wang
Ammonia is considered as a potential hydrogen carrier as its high hydrogen content. Hydrogen release still presents challenges due to the lack of efficient catalyst. In this work, we report a Ni@SiO 2 catalyst prepared through a sol–gel method, which displays satisfied catalytic activity and remarkable long-term stability. The origination of activity and stability has been investigated carefully by various characterizations. The strong interaction between nickel species and silica species is responsible for the excellent performance via generating small nickel particle and hindering the sintering of nickel during the high temperature reaction condition. This study offers novel insights into the design and preparation of highly efficient catalysts for ammonia decomposition to produce hydrogen.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Junyu Wang,Jiangnan Guo,Qinggang Zhou,Yuejin Zhu,Qizhi Liu,Shuozhen Hu,Xinsheng Zhang
Formic acid is a desirable liquid hydrogen storage compound for solving transport and storage problems of hydrogen for onboard fuel cells. Optimizing adsorption/desorption energy of intermediates can directly modulate the performance of Pd catalysts in formic acid dehydrogenation (FAD). Herein, we introduce internal electric field with controllable strength to regulate the adsorption/desorption of intermediates on Pd. Non-ferroelectric cubic-phase barium titanate (CBT) is heat-treated at high temperature to obtain ferroelectric tetragonal-phase barium titanate (TBT(C)), which exhibits internal electric field. The strength of the internal electric field is successfully adjusted by heat treatment at different temperatures. The size of Pd nanoparticles is restricted between 2.2 and 2.7 nm, and the electronic effect of Pd is effectively eliminated by coating TBT(C) with mesoporous carbon shell (TBT(C)@SC). Experimental results prove that the internal electric field promotes the desorption of hydrogen on Pd. Pd/TBT(C)@SC-800 obtained by heat treatment at 800 °C, with the optimal internal electric field strength, exhibits high activity and hydrogen selectivity for FAD. This work provides a new strategy for designing FAD catalysts.
研究领域:
化学
·
材料科学
·
催化反应
✓ 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）