Small
·
2024
·
IF 13
Wenxuan Zhang,Linming Zhou,Xin Zhang,Zhenguo Huang,Fang Fang,Zijian Hong,Juan Li,Mingxia Gao,Wenping Sun,Hongge Pan,Yongfeng Liu
Nanostructured metal hydrides with unique morphology and improved hydrogen storage properties have attracted intense interests. However, the study of the growth process of highly active borohydrides remains challenging. Herein, for the first time the synthesis of LiBH 4 nanorods through a hydrogen-assisted one-pot solvothermal reaction is reported. Reaction of n-butyl lithium with triethylamine borane in n-hexane under 50 bar of H 2 at 40–100 °C gives rise to the formation of the [100]-oriented LiBH 4 nanorods with 500–800 nm in diameter, whose growth is driven by orientated attachment and ligand adsorption. The unique morphology enables the LiBH 4 nanorods to release hydrogen from ≈184 °C, 94 °C lower than the commercial sample (≈278 °C). Hydrogen release amounts to 13 wt% within 40 min at 450 °C with a stable cyclability, remarkably superior to the commercial LiBH 4 (≈9.1 wt%). More importantly, up to 180 °C reduction in the onset temperature of hydrogenation is successfully attained by the nanorod sample with respect to the commercial counterpart. The LiBH 4 nanorods show no foaming during dehydrogenation, which improves the hydrogen cycling performance. The new approach will shed light on the preparation of nanostructured metal borohydrides as advanced functional materials.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
W. Chen,L.Z. Ouyang,J.W. Liu,X.D. Yao,H. Wang,Z.W. Liu,M. Zhu
Sodium borohydride (NaBH 4 ) hydrolysis is a promising approach for hydrogen generation , but it is limited by high costs, low efficiency of recycling the by-product, and a lack of effective gravimetric storage methods. Here we demonstrate the regeneration of NaBH 4 by ball milling the by-product, NaBO 2 ·2H 2 O or NaBO 2 ·4H 2 O, with MgH 2 at room temperature and atmospheric pressure without any further post-treatment. Record yields of NaBH 4 at 90.0% for NaBO 2 ·2H 2 O and 88.3% for NaBO 2 ·4H 2 O are achieved. This process also produces hydrogen from the splitting of coordinate water in hydrated sodium metaborate. This compensates the need for extra hydrogen for generating MgH 2 . Accordingly, we conclude that our unique approach realizes an efficient and cost-effective closed loop system for hydrogen production and storage.
研究领域:
材料科学
·
化学工程
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2016
·
IF 3.014
Bao-Xia Dong,Long-Zheng Wang,Yun-Lei Teng,Zong-Wei Li,Juan Zhao
In this study, the superior effect of RbF on reducing the hydrogen desorption operating temperature of the Li N H system was demonstrated. By doping 5 mol% RbF in the LiNH 2 LiH system, we obtain the lowest hydrogen desorption peak temperature (211 °C) at a heating rate of 5 °C/min, which is approximately 69 °C lower than that of the pristine LiNH 2 LiH system. Moreover, the system starts to desorb H 2 at 120 °C, which is the lowest hydrogen desorption onset temperature. The hydrogen desorption peak and onset temperatures can be further decreased by doping more RbF. It is proposed that the RbH produced during heat treatment improves the dehydrogenation properties of the RbF-doped LiNH 2 LiH sample.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Qingyun Kang,Xiaofang Zhang,Qianyue Feng,Lin Zhang,Mingyu Chu,Chaoran Li,Panpan Xu,Muhan Cao,Le He,Qiao Zhang,Jinxing Chen
Hydro-depolymerization presents a promising avenue for transforming plastic waste into high-value hydrocarbons, offering significant potential for value-added recycling. However, a major challenge in this method arises from kinetic limitations due to insufficient hydrogen concentration near the active sites, requiring optimal catalytic performance only at higher hydrogen pressures. In this study, we address this hurdle by developing “hydrogen bubble catalysts” featuring Ru nanoparticles within mesoporous SBA-15 channels (Ru/SBA). The distinctive feature of Ru/SBA catalysts lies in their capacity for physical hydrogen storage and chemically reversible hydrogen spillover, ensuring a timely and ample hydrogen supply. Under identical reaction conditions, the catalytic activity of Ru/SBA surpassed that of Ru/SiO2 (no hydrogen storage capacity) by over 4-fold. This substantial enhancement in catalytic performance provides significant opportunities for near atmospheric pressure hydro-depolymerization of plastic waste.
研究领域:
材料科学
·
环境科学
·
化学工程
·
催化
✓ 已验证
DOI
PubMed
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
·
材料科学
·
纳米技术
·
氢能
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·Vol. 47
·期 83
·35352-35364
·
IF 7.139
Zhichao Yu,Wei Zhang,Yongxi Zhang,Yaokun Fu,Ying Cheng,Sanyang Guo,Yuan Li,Shumin Han
Magnesium hydroxide (MgH 2 ) has excellent reversibility and high capacity, and is one of the most promising materials for hydrogen storage in practical applications. However, it suffers from high dehydrogenation temperature and slow sorption kinetics. Rare earth hydrides and transition metals can both significantly improve the de/hydrogenation kinetics of MgH 2 . In this work, MgH 2 –Mg 2 NiH 4 –CeH 2.73 is in-situ synthesized by introducing Ni@CeO 2 into MgH 2 . The unique coating structure of Ni@CeO 2 facilitates homogeneous distribution of synergetic CeH 2.73 and Mg 2 NiH 4 catalytic sites in subsequent ball milling process. The as-fabricated composite MgH 2 -10 wt% Ni@CeO 2 powders possess superior hydrogenation/dehydrogenation characteristics, absorbing 4.1 wt% hydrogen within 60 min at 100 °C and releasing 5.44 wt% H 2 within 10 min at 350 °C. The apparent activation energy of MgH 2 -10 wt% Ni@CeO 2 is determined to be 84.8 kJ/mol and it has favorable hydrogen cycling stability with almost no decay in capacity after 10 cycles.
研究领域:
材料科学
·
无机化学
·
能源化学
·
纳米催化
·
氢能源存储
✓ 已验证
DOI
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Qingqing Li,Zhiwei Sun,Yilin Wei,Zixu Ma,Liucheng Wang,Renfeng Nie
Reversible hydrogen storage via Liquid organic hydrogen carriers (LOHCs) is one of the key technologies for efficient utilization of hydrogen energy. How to construct efficient dehydrogenation/hydrogenation catalysts that enable low-temperature catalysis still remains challenging. Herein, we present the design and construction of single-atom Co-N-C(x) catalysts allowing significantly improved acceptorless dehydrogenation of 1,2,3,4-tetrahydroquinoline (THQ). By varying the ligand/Co ratio, the optimal Co-N-C(1.5) can achieve 97.5% dehydrogenated product and 0.82 h −1 TOF value at ambient temperature, overperforming many reported non-noble metal even noble metal catalysts. This catalyst exhibits good recyclability and substrate versatility, enabling ambient temperature dehydrogenation of various N-heterocycles and efficient reverse hydrogenation of aromatic N-heterocycles, thus achieving the loop of reversible hydrogen storage. The active catalyst centers consist of specific Co-N x moieties and nitrogen species within the carbon support. Controlled experiments reveal that the different performance of Co-N-C(x) is determined by density of the Co-N x , and the rate-determining step of THQ dehydrogenation is correlated with the bond cleavages in surface-bound THQ. This work offers a promising pathway for energy-efficient and cost-effective hydrogen energy utilization under practical conditions.
研究领域:
催化化学
·
能源材料
·
氢能技术
✓ 已验证
产品关联
DOI
高影响因子
RARE METALS
·
2021
·Vol. 40
·期 11
·3195-3204
·
IF 4.003
Lu Zhi-Yu,Yu Hai-Jie,Lu Xiong,Song Meng-Chen,Wu Fu-Ying,Zheng Jia-Guang,Yuan Zhi-Fei,Zhang Liu-Ting
Magnesium hydride (MgH 2 ), which possesses high hydrogen density of 7.6 wt%, abundant resource and non-toxicity, has captured intense attention as one of the potential hydrogen storage materials. However, the practical application of Mg/MgH 2 system is suffering from high thermal stability, sluggish absorption and desorption kinetics. Herein, two-dimensional (2D) vanadium nanosheets (V NS ) were successfully prepared via a facile wet chemical ball milling method and proved to be highly effective on improving the hydrogen storage performance of MgH 2 . For instance, the MgH 2 + 7 wt% V NS composite began to release hydrogen at 187.2 °C, 152 °C lower than that of additive-free MgH 2 . At 300 °C, 6.3 wt% hydrogen was released from the MgH 2 + 7 wt% V NS composite within 10 min. In addition, the fully dehydrogenated sample could absorb hydrogen even at room temperature under hydrogen pressure of 3.2 MPa. X-ray diffractometer (XRD) and transmission electron microscopy (TEM) results confirmed metallic vanadium served as catalytic unit for facilitating the de/rehydrogenation reaction of MgH 2 . This finding presents an example of facile synthesis of two-dimensional (2D) vanadium with excellent catalysis, which may shed light on future design and preparation of highly effective layered catalysts for hydrogen storage and other energy-related areas.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2025
·
IF 9.1
Qiaoqi Li,Wenhao Xu,Kun Dai,Tengfei Miao,Yanlong Zou,Nianjia Wang,Xiaojun Sun,Xia Li,Lili Zhang
Sodium borohydride holds great promise as a stable hydrogen-rich carrier. However, hydrogen evolution reaction (HER) via NaBH 4 hydrolysis typically requires relatively high solution temperatures. Due to the elevated specific heat capacity of water, controlling the reaction temperature is not feasible, which leads to an uncontrollable hydrogen production rate and poses safety risks. This work proposes an innovative strategy for controllable photo-thermal synergistic catalysis by inducing the coexistence of photo-responsive and photo-thermal conversion cations within the framework of the catalyst through the high-entropy effect. A series of high-entropy Co 6- x Ni x FeAl 1- y Ga y -layered double hydroxides (CoNiFeAlGa-LDHs) were synthesized by hydrothermal method, exhibiting ultrafast photo-responsive catalytic capacity across a broad spectral range from 200 to 1500 nm. By controlling the illumination, CoNiFeAlGa-LDHs demonstrated exceptional on-demand HER capacity via NaBH 4 hydrolysis. Notably, the H 2 evolution rate of high-entropy Co 3 Ni 3 FeAl 0.5 Ga 0.5 -LDHs reaches 13.60 mol·g -1 ·h -1 and 2.76 mol·g -1 ·h -1 under full-spectrum and near-infrared irradiation, respectively. This surpasses the efficiency of most Co-based catalysts ever reported, presenting a novel approach to achieve for on-demand HER via NaBH 4 hydrolysis.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaoxia Chen,Cong Peng,Qingan Zhang
Magnesium hydride is a promising solid-state hydrogen storage material with a hydrogen capacity of 7.6 wt%. However, its practical applications are limited by high thermodynamic stability, sluggish desorption kinetics and poor cycling stability. To enhance the hydrogen desorption kinetics and cycling stability of MgH 2 , nanosized TiOF 2 and NbO 2 F are synthesized as catalytic additives in this work. After the preparation by ball milling and activation by de/hydrogenation cycling of MgH 2 –10 wt% TiOF 2 and MgH 2 –10 wt% NbO 2 F composites, the highly dispersed magnesium fluoride, magnesium-transition metal oxides and transition metal hydrides as well as multivalent transition metal species can be in-situ formed throughout the samples. Benefiting from the synergistic effect of these secondary phases, the two samples exhibit fast dehydrogenation kinetics with activation energies of 76.2 and 74.4 kJ mol −1 , respectively. It is noteworthy that the microstructure configurations can be preserved well after 50 cycles. Consequently, the dehydrogenation activation energies of the cycled samples only increase to 80.5 and 78.7 kJ mol −1 , respectively, showing good cycling stability. These results demonstrate that multivalent transition metal oxyfluorides can be used as efficient additives to improve hydrogen storage properties of MgH 2 .
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Zhongliang Ma,Jiguang Zhang,Yunfeng Zhu,Huaijun Lin,Yana Liu,Yao Zhang,Delong Zhu,Liquan Li
Metal nanocatalysis is an effective method to enhance the hydrogen storage properties of magnesium hydride (MgH2), and the catalytic effect can be further improved by a matrix material supported nanometal. In this work, carbon supported nano-Ni (Ni@C) was synthesized by calcination of dimethylglyoxime dinickel chelate, and then it was doped into MgH2 to improve the de/rehydrogenation kinetics. This shows that the homogeneously distributed Ni with refined particle size in carbon base leads to superior catalytic effects on hydrogen absorption/desorption of MgH2-5 wt % Ni@C. The MgH2-5 wt % Ni@C starts to desorb hydrogen at 187 °C, which is 113 °C lower than that of as-milled MgH2. Moreover, it takes only 500 s to thoroughly desorb hydrogen at 300 °C, which is 3000 s faster than as-milled MgH2 under the same dehydrogenation conditions. According to the Kissinger’s method, the apparent activation energy for desorption of the MgH2-5 wt % Ni@C is 66.5 ± 1.8 kJ mol–1, which is about 79.9 kJ mol–1 lower than that of as-milled MgH2. Cycling experiments show that the capacity retentions of hydrogen absorption and desorption after 10 cycles at 275 °C are 91% and 93%, respectively. Transmission electron microscope analysis shows that part of Ni transformed to Mg2NiH4/Mg2Ni during hydrogen absorption/desorption cycles.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
危险品化学品经营许可证（带存储）