JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Tianping Huang,Jianxin Zou,Ning Zhao,Xiaoqin Zeng,Wenjiang Ding
A new reversible hydrogen storage system, 3NaBH 4 -0.5ScF 3 -0.5YF 3 , was synthesized by using the ball-milling method. It is shown that no reaction occurs during the ball-milling process. The hydrogen desorption process of the ball-milled composite can be divided into three consecutive steps: (i) An initial stage from room temperature to 320 °C with about 0.42 wt% of hydrogen released, that can be ascribed to the substitution of H − by F − in NaBH 4 ; (ii) The second stage starts from 320 °C to 450 °C, releasing about 1.06 wt% of hydrogen; (iii) The final stage ranges from 450 °C to 480 °C, with 2.58 wt% of hydrogen released. The total yield of hydrogen reaches 4.06 wt% at 480 °C. The completely dehydrogenated products of the 3NaBH 4 -0.5ScF 3 -0.5YF 3 composite can absorb 2.15 wt% of hydrogen at 380 °C in 6.5 h, which shows greatly enhanced reversibility when compared with sole ScF 3 addition. It should be noted that one of the destabilizers ScF 3 was also regenerated besides NaBH 4 in the rehydrogenated products. Based on the XRD and FTIR analyses, the synergistic effects of 3d transition metal fluoride ScF 3 and rare earth metal fluoride YF 3 on the hydrogen desorption and absorption performance of NaBH 4 were discussed.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Jiajing Zhu,Hui Wang,Liangjun Huang,Liuzhang Ouyang,Lan Zhang,Min Zhu
Nanosized SrTiO3, a common photocatalyst that enhances water splitting for hydrogen production, has been synthesized to catalyze the reversible hydrogen gas–solid reaction of MgH2. Compared to the pure MgH2, the milled MgH2-SrTiO3 composite shows significantly enhanced hydrogen storage properties, absorbing 3.5 wt % H2 within 1 min at room temperature and releasing 6.1 wt % H2 within 9 min at 250 °C. The activation energy for dehydrogenation is 82.91 kJ/mol, which is 52.09 kJ/mol lower than that of as-milled MgH2. The composite retains a capacity of 5.47 wt % after 40 cycles of dehydrogenation at 250 °C. The catalytic mechanism of nanosized SrTiO3 was discussed. Therefore, like anatase TiO2 photocatalysts, SrTiO3 shows an excellent catalytic effect to enhance the hydrogen sorption of MgH2 at significantly lower temperatures. A significant number of photocatalytsts have great potential to enhance the hydrogen sorption of Mg, making them promising candidates for solid-state hydrogen storage materials.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 26
·11164-11171
·
IF 3.288
Zhuo Wang,Jin Liu,Zhen Li,Xianbiao Wang,Ping Wang,Di Wang,Fengjun Zhang
A crosslinkable UIO-66 type MOF material denoted UIO-66-DETA composed of Zr(IV) metal ions and 2,5-diallyl ether terephthalic acid (DETA) was synthesized, and then by initiating double bond crosslinking, a new crosslinking MOF material denoted UIO-66-DETA-CL was obtained. UIO-66-DETA and UIO-66-DETA-CL were characterized by FTIR spectroscopy, PXRD, 1H solid-state NMR spectroscopy, SEM, nitrogen sorption, thermogravimetric analysis and hydrogen storage tests to analyze their structure and properties. The results showed that a crosslinked structure has been formed, and UIO-66-DETA-CL can maintain its structure below 340 °C, compared with UIO-66-DETA; its carbon residual rate is improved, which shows that the crosslinking modification enhances the thermal stability. Meanwhile, the hydrogen uptake capacity of UIO-66-DETA-CL reaches 5.36 wt% at 77 K and 4 MPa. Furthermore, the hydrogen adsorption enthalpy of UIO-66-DETA-CL (ΔHUIO-66-DETA-CL) calculated using the Arrhenius equation reaches −0.889 kJ mol−1, which is significantly improved by crosslinking modification. The crosslinked structure changes the pore size and increases the active adsorption sites in organic ligands. The framework of UIO-66-DETA-CL can provide more polar charges to cause some hydrogen molecules to be negatively charged because of a small HOMO–LUMO gap, and a lower LUMO energy level of UIO-66-DETA-CL enables stronger negative charge acceptability. Therefore, crosslinking modification enhances the material's hydrogen storage capacity. This result provides a new idea for the crosslinking modification of MOFs.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 9
·1745
·
IF 4.324
Ze Sun,Liuting Zhang,Nianhua Yan,Jiaguang Zheng,Ting Bian,Zongming Yang,Shichuan Su
Magnesium hydride (MgH2) has been considered as a potential material for storing hydrogen, but its practical application is still hindered by the kinetic and thermodynamic obstacles. Herein, Mn-based catalysts (MnCl2and Mn) are adopted and doped into MgH2to improve its hydrogen storage performance. The onset dehydrogenation temperatures of MnCl2and submicron-Mn-doped MgH2are reduced to 225 °C and 183 °C, while the un-doped MgH2starts to release hydrogen at 315 °C. Further study reveals that 10 wt% of Mn is the better doping amount and the MgH2+ 10 wt% submicron-Mn composite can quickly release 6.6 wt% hydrogen in 8 min at 300 °C. For hydrogenation, the completely dehydrogenated composite starts to absorb hydrogen even at room temperature and almost 3.0 wt% H2can be rehydrogenated in 30 min under 3 MPa hydrogen at 100 °C. Additionally, the activation energy of hydrogenation reaction for the modified MgH2composite significantly decreases to 17.3 ± 0.4 kJ/mol, which is much lower than that of the primitive MgH2. Furthermore, the submicron-Mn-doped sample presents favorable cycling stability in 20 cycles, providing a good reference for designing and constructing efficient solid-state hydrogen storage systems for future application.Keywords:hydrogen storage;MgH2;Mn-based catalysts;catalytic effect;reversibility
研究领域:
材料科学
·
化学工程
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Energy Technology
·
2017
·Vol. 5
·期 8
·1399-1406
·
IF 2.789
Zhong Ma,Rui Xiao,Huiyan Zhang
A technology for hydrogen storage is proposed based on the repeated reduction of magnetite (Fe 3 O 4 +4 H 2 →3 Fe+4 H 2 O) and the oxidization of metallic iron (3 Fe+4 H 2 O→Fe 3 O 4 +4 H 2 ). Herein, we prepared three montmorillonite (MMT)-supported iron oxide samples by using a sol–gel method and demonstrated their application in hydrogen storage through a chemical looping process. The redox performance of the Fe-MMT samples was studied at 600 °C in a fixed-bed reactor. The results showed that 70 Fe-MMT (with 70 wt % Fe 2 O 3 ) exhibited relatively good redox performance owing to its excellent anti-agglomeration ability and sintering resistance. After the redox performance tests, Fe 2 SiO 4 was observed in all Fe-MMT samples. It was worth noting that the diffraction intensity of Fe 2 SiO 4 in 70 Fe-MMT was much weaker than in 30 Fe-MMT (30 wt % Fe 2 O 3 ) and 50 Fe-MMT (50 wt % Fe 2 O 3 ), which was owed to the high MMT content in the 30 Fe-MMT and 50 Fe-MMT samples. The formation of Fe 2 SiO 4 in repeated redox cycles could reduce the stability and recyclability of Fe-MMT samples. This might be the major reason for the better hydrogen storage performance of 70 Fe-MMT compared with 30 Fe-MMT and 50 Fe-MMT.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 34
·9752-9759
·
IF 0
Xiulin Fan,Xuezhang Xiao,Lixin Chen,Liuting Zhang,Jie Shao,Shouquan Li,Hongwei Ge,Qidong Wang
NaAlH4, a prototypical high energy density complex hydride, possesses a favorable thermodynamics and high hydrogen storage capacity. However, the poor kinetics and degradation of cycling stability retard its practical application. To ease these problems, CeB6, CeF3 and CeO2 nanoparticles with a size of about 10 nm are synthesized by the wet-chemistry method and introduced into NaAlH4 systems as additives in this work. The results show that all of the nanoparticles are effective in improving the hydriding–dehydriding kinetics of NaAlH4, and nano-CeB6 possesses the highest catalytic activity. The rehydrogenation of dehydrogenated NaAlH4 doped with nano-CeB6 can be accomplished in less than 20 min with a high capacity of 4.9 wt%, which shows a 20% increase in capacity compared to that of chloride-doped NaAlH4. Due to the structural stability and good dispersion of nano-CeB6 and nano-CeF3, a favorable cycling stability with high capacity retention is achieved for their doped samples. Moreover, hydrogen can be released from the hydrogenated sample doped with nano-CeB6 at a temperature as low as 75 °C, fulfilling the operation temperature of a PEM fuel cell. In the nano-CeO2 doped NaAlH4 system, CeO2 is first reduced to CeH2.51. In the subsequent cycles, the formed CeH2.51 gradually transforms into Ce–Al, and simultaneously the kinetics of the doped system is further enhanced. It is believed that the utilization of Ce-based nanoparticles as catalysts would substantially improve the practical applications of NaAlH4 for hydrogen storage.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 44
·20279-20285
·
IF 3.3
Xiaoqian Peng,Jing Zhang,Xu Zhang,Xiaochan Liu,Zhiqiang Huang,Haibo Li,Xibin Yi
Hydrogen is regarded as one of the most promising energy sources of the future, due to its low-cost, zero-pollution, and high-heat value. Nevertheless, traditional methods of storing hydrogen are commonly accompanied by the risk of leaks and explosions, so how to store and transport hydrogen safely and efficiently is a critical issue that needs to be addressed. Solid-state hydrogen storage is the most attractive way to store hydrogen in nanomaterials by chemical or physical adsorption, which has the advantages of high energy density and good safety. Here, a rational Ni–Zn bimetallic MOF has been constructed by a straightforward synthetic technique, in which the Zn atom was partially replaced by the Ni atom. The micropore rate of the Ni–Zn bimetallic MOFs is higher than that of ZIF-8. In addition, the presence of Ni provides more unsaturated metal sites and strengthens the bonding between hydrogen molecules and Ni, effectively improving the hydrogen storage capacity of Ni–Zn bimetallic MOFs. The experimental results show that the hydrogen adsorption capacity of Ni–Zn bimetallic MOFs can reach 1.35 wt% at 77 K and 1 bar.
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
ACS Catalysis
·
2022
·
IF 13.7
Shuchao Jiang,Junxia Yang,Shengliang Zhai,Ling Zhang,Rui Tu,Tie Yu,Dong Zhai,Lei Sun,Weiqiao Deng,Guoqing Ren
Formic acid (FA)/formate as a promising liquid organic hydrogen carrier exhibits great potential for future energy supplies. However, FA/formate-based hydrogen storage and release, which can be operated under ambient conditions, is challenging but attractive. Here, we report an ambient hydrogen storage and release process that uses the acidity and alkalinity of the reaction solution to control hydrogen production or consumption via an l-arginine-functionalized active carbon-supported PdAu alloy catalyst (PdAu/AC-LA). By regulating the LA loading and Pd/Au ratio, we obtain the optimal catalytic activity with turnover frequency (TOF) of 1760 h–1 for FA dehydrogenation under acidic conditions and 138 h–1 for CO2 hydrogenation under alkaline conditions. Comprehensive characterizations, including X-ray photoelectron spectroscopy (XPS), CO2 temperature-programmed desorption (CO2-TPD), and HCOO– adsorption experiments, reveal that the synergistic effect between PdAu alloy and strongly basic l-arginine enhances catalytic activity by regulating the adsorption of reactants. Our work, as a successful example of FA/formate-based hydrogen storage and release under ambient conditions, may aid putting the safe and energy-saving use of hydrogen into practice.
研究领域:
化学工程
·
催化科学
·
能源技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yaning Kong,Fei Wang,Guodong Zhang,Xiaolin Wang
It is anticipated to achieve safe, economical, and high-density hydrogen storage via hydrate, but sluggish formation kinetics of H 2 hydrate and low hydrogen storage capacity limit its application, and appropriate kinetic promoters are required to improve the situation. In this work, three nano promoters were prepared by soap-free emulsion polymerization method, the functional groups of -SO 3 − , –COO − and -N(CH 3 ) 3 + were separately immobilized on nano spheres to produce the nano promoters of -SO 3 − @PSNS, –COO − @PSNS and -N(CH 3 ) 3 + @PSNS, and their influence on the formation kinetics of mixed H 2 /THF hydrate was evaluated, while the performance of conventional kinetic promoters of methane hydrate was also estimated for comparison. It was found that the formation kinetics of mixed H 2 /THF hydrate was enhanced in the presence of nano promoters, which improve early growth of H 2 /THF hydrate and later water-to-hydrate conversion, leading to large hydrogen storage capacity. -SO 3 − @PSNS causes H 2 /THF hydrate to be looser and performs the best among the three nano promoters, hydrogen storage capacity in -SO 3 − @PSNS system is up to 0.467 wt% at 12 MPa, which increase by 39.8% comparing with that in pure THF system, and satisfactory hydrogen storage capacity of 0.303 wt% was also obtained under milder condition (7 MPa). For conventional kinetic promoters, L-methionine performs the best and shows similar promotion effect like -SO 3 − @PSNS, but it is excluded for large-scale industrial application when taking its high cost and perishable nature into consideration, whereas this scenario is improved by the proposed nano promoters.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xingyu Liu,Shaoyang Shen,Yunqi Jia,Lin Jiang,Liuzhang Ouyang
Hydrogen is a clean, sustainable, and efficient energy carrier. However, achieving safe and controllable storage for practical applications remains a challenge. The practical applications of lithium borohydride remain challenging due to its violent hydrolysis reaction. Herein, we report the synthesis of bimetallic hydrogen storage materials based on LiK(BH4)2 (LKBH-x-1) through ball-milling various ratios of potassium borohydride and lithium borohydride, which demonstrate excellent stability in aqueous solutions and extremely high hydrogen storage capacity. Optimizing reaction conditions indicated that the LKBH-4-1 produced from a 4:1 ratio exhibited an exceptionally high theoretical hydrogen storage capacity of 14.3 wt % while retaining excellent stability in aqueous solutions at ambient conditions. Further density functional theory (DFT) calculations revealed that the stability of LKBH-x-1 in aqueous solution is attributed to the robustness of B–H bonds in the differing phases. Furthermore, we clarify the feasibility of the LKBH-x-1 regeneration cycle by ball milling MgH2 and the hydrolysis products of LKBH-x-1. This work provides a new perspective for regulating borohydride hydrolysis for hydrogen production.
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xue Gao,Yuchen Mao,Zeming Zhong,Liangjun Huang,Hui Wang,Min Zhu
Porous carbon materials (PCMs) with high specific surface area (SSA) exhibit significant potential for hydrogen storage applications but are severely limited due to the weak interactions of H 2 . In this work, polyvinylpyrrolidone (PVP) was employed to prepare PCMs with ultra-high SSA and high micropore ratio through applying mechanical pressure before activation. This approach resulted in an SSA exceeding 3100 m 2 /g and a maximum S BET /S Micro ratio above 90%. The increased microporosity significantly improved hydrogen storage performance, with a 62% increase in hydrogen uptake capacity per SSA at 77 K and 50 bar-H 2 , suggesting the strengthened interaction between PCMs and H 2 . This is further supported by the increased isosteric heat of hydrogen adsorption (Q st ) values from 6.93 to 7.56 kJ/mol at near-zero hydrogen coverage, with S Micro /S BET increasing from 75.86% to 90.83%. Moreover, the increased microporosity enhances the volumetric and usable hydrogen storage capacity. Remarkably, the PCM with 84.35% microporosity and high SSA of 3116.58 m 2 /g exhibits a hydrogen uptake of 6.10 wt% (26.47 g/L) at 77 K under 50 bar-H 2 , and retains 1.26 wt% (5.52 g/L) even at 298 K and 130 bar-H 2 . This study provides a valuable reference for the large-scale preparation of PCMs with high SSA and microporosity for hydrogen storage.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）