CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 35
·9087-9093
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IF 5.236
Yongyang Zhu,Hao Zhong,Hui Wang,Liuzhang Ouyang,Jiangwen Liu,Zhenguo Huang,Min Zhu
Graphical A cost-effective way to produce NaBH 4 with high yield by ball milling hydrated borax (Na 2 B 4 O 7 ⋅ 10H 2 O) with cheap Al or Al 88 Si 12 at ambient condition is presented. An effective strategy was developed to facilitate mass transfer during the reaction by introducing NaH to enable the formation of loose NaAlO 2 instead of dense Al 2 O 3 on Al surface, and by using Si as a milling additive that prevents agglomeration and also breaks up passivation layers. A significant obstacle in the large-scale applications of sodium borohydride (NaBH 4 ) for hydrogen storage is its high cost. Herein, we report a new method to synthesize NaBH 4 by ball milling hydrated sodium tetraborate (Na 2 B 4 O 7 ⋅ 10H 2 O) with low-cost Al or Al 88 Si 12 , instead of Na, Mg or Ca. An effective strategy is developed to facilitate mass transfer during the reaction by introducing NaH to enable the formation of NaAlO 2 instead of dense Al 2 O 3 on Al surface, and by using Si as a milling additive to prevent agglomeration and also break up passivation layers. Another advantage of this process is that hydrogen in Na 2 B 4 O 7 ⋅ 10H 2 O serves as a hydrogen source for NaBH 4 generation. Considering the low cost of the starting materials and simplicity in operation, our studies demonstrate the potential of producing NaBH 4 in a more economical way than the commercial process.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Hao Zhong,Liuzhang Ouyang,Jiangwen Liu,Chenghong Peng,Xiaoke Zhu,Weiheng Zhu,Fang Fang,Min Zhu
Irreversibility negatively impacts the application of NaBH 4 hydrolysis for hydrogen generation . Byproduct regeneration is key to solving this issue. In this work, the direct byproduct of aqueous NaBH 4 hydrolysis, NaBO 2 ·4H 2 O, is reacted with Mg 2 Si to regenerate NaBH 4 via ball milling at room temperature under an argon atmosphere . In this process, the H − in NaBH 4 is exclusively from the H + in NaBO 2 ·4H 2 O. The regenerated NaBH 4 , with a maximum yield of 74%, has the same physicochemical properties as a commercial sample. We also demonstrate that Mg 2 Si reacts with NaBO 2 ·4H 2 O to generate NaBO 2 ·2H 2 O, followed by a direct reaction between the residual Mg 2 Si and NaBO 2 ·2H 2 O to produce NaBH 4 . The energy efficiency of this method is approximately 40%.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Miaojun Huang,Hao Zhong,Liuzhang Ouyang,Chenghong Peng,Xiaoke Zhu,Weiheng Zhu,Fang Fang,Min Zhu
The application of NaBH 4 hydrolysis to hydrogen generation is currently obstructed by its regeneration. Finding a simple and low cost method to regenerate its hydrolysis byproduct is therefore important. Herein, the regeneration of NaBH 4 is obtained by reacting its direct hydrolysis byproduct, NaBO 2 ·2H 2 O, with a mixture of Mg and Mg 2 Si by ball milling. In this reaction, the reduced agents are only metal and intermetallic compounds , thus hydrogen in the regenerated NaBH 4 (H δ− ) derives solely from NaBO 2 ·2H 2 O (H δ+ ). The introduction of Mg 2 Si increases the NaBH 4 regeneration yield to 86%, which is the highest regeneration yield reported for NaBH 4 until now. The reaction mechanism was also clarified for the first time.
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
·
2019
·
IF 4.084
Chenglei Qin,Liuzhang Ouyang,Hui Wang,Jiangwen Liu,Huaiyu Shao,Min Zhu
Sodium borohydride (NaBH 4 ) is considered to be an excellent hydrogen-generation material via hydrolysis. However, it remains challenge to regenerate it after hydrolysis in practical applications. Therefore, a low-cost regeneration method from hydrolysis by-products for recycling is the key issue. In this study, NaBH 4 was successfully regenerated by direct high-energy ball milling of magnesium alloy (Mg 17 Al 12 ) and hydrolysis by-product NaBO 2 ·2H 2 O with addition of a small amount of NaH. Notably, unlike traditional method, here there is no need of adding extra hydrogen and the H − in the regenerated NaBH 4 is mainly from the H + in the coordinated water. It was found that through adding a small amount of NaH, the highest yield may reach 57% after optimizing the regeneration process. In addition, it is the first time we found that not only Mg can participate in the reaction, but also Al; and the addition of NaH can promote the reaction. Furthermore, the regeneration mechanism of NaBH 4 was analyzed and the transition pattern [B(OH) 4 ] − /[BH 3 (OH)] − /[BH 4 ] − was successfully observed during the regeneration process. It is worth emphasizing that NaBH 4 can be regenerated through ball milling method, which is energy-saving and suitable for up-scaling in the future.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
·
2020
·
IF 3.693
Xi Senliang,Wang Xiaojun,Wu Dan,Hu Xingtao,Zhou Shixue,Yu Hao
Phosphotungstic acid (HPW) as a polyoxometalate was selected as the active component of the catalyst. The activated carbon supported different percentage of HPW catalysts were prepared by impregnation and were characterized by X-ray diffraction (XRD), nitrogen adsorption, Fourier transform infrared (FTIR), and scanning electron microscope (SEM). The results showed that the HPW retained the original Keggin structure after being supported on activated carbon, the specific surface of the HPW/C was much bigger than that of pure HPW. The catalytic performance of HPW/C in the hydrogen generation reaction by hydrolysis of sodium borohydride in seawater and in deionized water were studied. 2.5 wt.% HPW/C showed the fastest hydrolysis reaction rate and the biggest volume of hydrogen generated. As for hydrolysis of sodium borohydride, catalytic effect of HPW/C was better in seawater than in distilled water. HPW dispersed on activated carbon is a real promising catalytic system for the development of hydrogen generation by hydrolysis of NaBH4 in seawater.
研究领域:
化学
·
材料科学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Wenlong Chen,Yuting Chen,Runwei Mo,Jiannong Wang
To reduce the amount of carbon dioxide (CO 2 ) already emitted into the atmosphere, various carbon capture, utilization, and storage (CCUS) technologies have been developed for climate and economic reasons in recent years. However, the state of art CCUS techniques suffer from deficiencies such as high cost, low yield, and harsh and discontinuous production conditions. In this work, we report a new thermal reduction method for continuously conversing CO 2 to methane (CH 4 ) by introducing sodium borohydride (NaBH 4 ) as a reductant under catalyst-free conditions. Experimental results show that CO 2 can be fully captured and converted to CH 4 and carbon monoxide (CO) and the selectivity efficiency of CO 2 to CH 4 can be achieved to be as high as 90% with the optimization of experimental conditions. Such a result originates from the high activity of NaBH 4 and high selectivity of the thermal reduction of CO 2 . To demonstrate one of the potential usages of the reduction products, we integrated the thermal reduction of CO 2 with the production of carbon nanotubes (CNTs). As long as CO 2 is supplied at the source end, the reduction products can undergo catalytic decomposition to produce a CNT fiber or film continuously at the final end. The present technique is featured with simple equipment setup, low cost, and continuous thermal reduction, thus providing a new pathway for the large-scale conversion of CO 2 into high-valued products for wide applications.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 17
·10723-10728
·
IF 10.733
Hao Zhong,Liuzhang Ouyang,Meiqin Zeng,Jiangwen Liu,Hui Wang,Huaiyu Shao,Michael Felderhoff,Min Zhu
The regeneration of sodium borohydride (NaBH4) is crucial to form a closed cycle after it either supplies hydrogen energy via a hydrolysis process or provides energy through electron transfer at the anode of direct borohydride fuel cells (DBFCs). In both of these cases, the spent fuels are NaB(OH)4 from NaBO2 aqueous solution. However, the current regeneration process from (NaB(OH)4)·xH2O to form NaBH4 by reduction reaction and calcination at high temperature with metal hydrides as reducing agents is very expensive. In this work, we developed a simple regeneration process via ball milling with Mg–Al alloys as the reducing agent for NaB(OH)4 under an argon atmosphere. Under optimized conditions, a high yield of about 72% of NaBH4 could be obtained. Mechanistic study showed that all the hydrogen atoms from NaB(OH)4 remain in NaBH4 and no additional hydrogen sources are needed for the reduction process. The inexpensive Mg–Al alloy works as a reducing agent transforming the H+ to H− in NaBH4. This approach demonstrates a ∼20-fold cost reduction compared with the method using metal hydrides. This opens the door to the commercial implementation of simple ball milling processes for the regeneration of spent NaBH4 from NaB(OH)4 with cheap reducing agents.
研究领域:
化学工程
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
Chemical Engineering and Processing-Process Intensification
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2020
·
IF 3.731
Chenhua Shu,Faying Lai,Feng Zhu,Dan Luo
In order to lower desulfurization cost, the NaBH 4 preparation via NaBO 2 electroreduction was introduced into the integrated process of extraction and reductive desulfurization. Accordingly, a novel desulfurization method was developed where NaBH 4 can be recycled at the same time as desulfurization. The process of NaBH 4 preparation via NaBO 2 electroreduction was analyzed by cyclic voltammetry and the effect of pulse parameters on desulfurization efficiency was optimized by orthogonal experiments. Under optimal conditions desulfurization efficiency of more than 97 % was obtained for model fuel oil. Desulfurization mechanism and kinetics was probed. Results showed that the desulfurization of DBT should proceed over direct cleavage of C S bond and desulfurization reaction could be treated as pseudo-first-order reaction. Furthermore, the structures of original and recycled ionic liquids (ILs) were analyzed by nuclear magnetic resonance and the desulfurization performance of the recycled ILs was also investigated. Results showed that ILs maintained their original structures after regeneration and displayed good reusability. In summary, the novel desulfurization process is feasible and promising.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Chenhua Shu,Tonghua Sun,Jinping Jia,Ziyang Lou
A novel integrated process was proposed for reductive desulfurization of diesel fuel, in which the reductant sodium borohydride (NaBH4) was in situ generated via sodium metaborate (NaBO2) electroreduction. In order to improve the conversion rate of BO2– into BH4–, NaBO2 electroreduction was fulfilled by applying pulse voltage and using a boron-doped diamond (BDD) thin film electrode. The NaBO2 electroreduction process was analyzed by cyclic voltammetry and 11boron nuclear magnetic resonance (11B NMR) and the factors that influenced desulfurization efficiency were investigated. Under the optimal conditions desulfurization efficiency reached more than 93% for model diesel fuel. The components of model diesel fuel after desulfurization were analyzed by gas chromatography/mass spectrometry (GC/MS) and the electrolyte and digestion solution of precipitate were analyzed by inductively coupled plasma (ICP). Results indicated that B recycle was realized at the same time as desulfurization. Finally, the desulfurization of real diesel fuel was investigated. This work showed that the integrated process may be a new option for desulfurization of diesel fuel due to its mild conditions.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Chunhui Yue,Pan Yang,Jingchuan Wang,Xiaochong Zhao,Yuqi Wang,Lijun Yang
Development of low-cost and high-efficiency catalysts for hydrogen generation represents the significant challenge for realizing hydrogen economy. NiCo and nano-Pd loaded NiCo microfibers with high surface area has been successfully developed by electrospinning and following vacuum thermal treatment. Towards hydrogen generation, the catalyst exhibits efficient TOF as high as 350 and 680 mL min −1 gcat −1 for NiCo and nano-Pd loaded NiCo microfibers, providing superior performance compared with the most promising reported catalysts. The excellent catalytic activity remain above 90% confirming the remarkable durability. The insights uncovered here inspire and guide the rational design of advanced catalysts for the rapidly developing hydrogen energy applications.
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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Hao Zhong,Kang Chen,Chenglei Qin,Chengguang Lang,Jiangwen Liu,Hui Wang,Junrui Zhang,Liuzhang Ouyang
Onsite hydrogen generation by sodium borohydride hydrolysis resolves hydrogen energy supply system challenges. However, the spent-NaBH 4 regeneration is still a problem in the closed loop of this irreversible reaction. As the by-product is the key to the problem, NaB(OH) 4 is regarded as not the boron source but the hydrogen source of NaBH 4 regeneration. Therefore, in this study, inexpensive Al metal and NaB(OH) 4 are ball milled under argon to regenerate NaBH 4 without additional hydrogen input. However, the ball-milling reaction is hindered by the flexible Al and impact oxide layer, and the NaBH 4 yield is only approximately 22 %. Therefore, a brittle intermetallic compound Mg 2 Al 3 is reacted with NaB(OH) 4 by ball milling, achieving a NaBH 4 yield of over 42 %. The mechanism study shows that the brittleness of the raw material plays an important role in promoting the ball-milling reaction. This study achieves NaBH 4 regeneration using only Al as the reducing agent and provides a promising method to promote the mechanochemical regeneration of NaBH 4 .
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 Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Yongyang Zhu,Liuzhang Ouyang,Hao Zhong,Jiangwen Liu,Hui Wang,Huaiyu Shao,Zhenguo Huang,Min Zhu
Sodium borohydride (NaBH4) has been identified as one of the most promising hydrogen storage materials; however, it is still challenging to produce NaBH4 with low cost and high efficiency, which are largely determined by the sources of boron and hydrogen and reducing agents used. Herein, we report an economical method to produce NaBH4 by ball milling hydrated borax (Na2B4O7·10H2O and/or Na2B4O7·5H2O) with different reducing agents such as MgH2, Mg, and NaH under ambient conditions. The direct use of natural hydrated borax avoids the dehydration process (at 600 °C) and consequently reduces cost and improves overall energy efficiency. A high yield of 93.1% can be achieved for a short ball mill duration (3.5 h) for Na2B4O7·5H2O-NaH-MgH2 system. In this system, H2 is generated in situ which subsequently reacts with Mg forming MgH2. Low cost Mg is therefore employed to replace the majority of MgH2, leading to an attractive yield of 78.6%. To further reduce the cost of raw materials and improve the utilization of hydrogen source in the hydrated borax, Na2B4O7·10H2O is used to partially substitute for Na2B4O7·5H2O, leading to a complete replacement of MgH2. Compared with literature results, the optimized recipe features low cost and high efficiency since it utilizes hydrogen from the hydrated water in natural borax and avoids high temperatures. Our finding is expected to facilitate applications of NaBH4 for hydrogen storage.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）