Article
Chemistry, Inorganic & Nuclear
Noemi Leick, Ba L. Tran, Mark E. Bowden, Thomas Gennett, Tom Autrey
Summary: This study investigated the thermal stability of coordination complexes formed between different glymes with Mg(BH4)(2), revealing diverse phase transitions, speciations, and decomposition pathways despite their structural similarities.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Nicholas A. Strange, Noemi Leick, Sarah Shulda, Andreas Schneemann, Vitalie Stavila, Andrew S. Lipton, Michael F. Toney, Thomas Gennett, Steven T. Christensen
Summary: Magnesium borohydride is a promising material for hydrogen storage, but its slow dehydrogenation kinetics and formation of intermediate polyboranes limit its application in clean energy technologies. This study presents a novel approach of modifying the physicochemical properties of magnesium borohydride by adding reactive molecules in the vapor phase. The effects of four different molecules on the additive-Mg(BH4)(2) interaction and hydrogen release at lower temperatures are examined. The results demonstrate the efficacy of this approach and provide a new path for additive-based modification of hydrogen storage materials.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Engineering, Environmental
Yongyang Zhu, Shaoyang Shen, Liuzhang Ouyang, Jiangwen Liu, Hui Wang, Zhenguo Huang, Min Zhu
Summary: This study reports an economical method to synthesize Mg(BH4)(2) by converting B-O bonds in widely available borates or boric acid to B-H. This method avoids expensive boron sources and high pressure and temperature conditions, significantly reducing costs, and could be an alternative to the current synthesis processes of Mg(BH4)(2).
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
J. L. Snider, T. M. Mattox, Y-S Liu, L. F. Wan, P. Wijeratne, M. D. Allendorf, V Stavila, B. C. Wood, L. E. Klebanoff
Summary: LiH significantly improves the hydrogenation of MgB2, lowering the temperature and without forming undesirable intermediates, while TiH2 is essentially inert when mixed with MgB2 during high-pressure hydrogenation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
Xuancheng Wang, Xuezhang Xiao, Jiaguang Zheng, Zhouming Hang, Wenping Lin, Zhendong Yao, Meng Zhang, Lixin Chen
Summary: The study shows that ball-milling magnesium borohydride with titanium nano-particles results in enhanced hydrogen release, improved dehydrogenation kinetics, and lower activation energy. The catalyzed magnesium borohydride also exhibits high reversibility during partial dehydrogenation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
J. L. Snider, T. M. Mattox, Y-S Liu, L. F. Wan, P. Wijeratne, M. D. Allendorf, V Stavila, B. C. Wood, L. E. Klebanoff
Summary: The study reveals that LiH/MgB2 and TiH2 have different effects on the hydrogen storage properties of MgB2, with LiH/MgB2 showing higher reactivity in the surface and near-surface regions, while TiH2 does not significantly aid MgB2 hydrogenation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
Robert T. Bell, Nicholas A. Strange, Noemi Leick, Vitalie Stavila, Mark E. Bowden, Tom S. Autrey, Thomas Gennett
Summary: The use of an organic borohydride salt additive, tetramethylammonium borohydride (TMAB), has been shown to enhance the chemical stability and thermal cyclability of Mg(BH4)(2) melt. This finding is significant for applications in hydrogen storage and magnesium battery technologies.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
V. V. Berezovets, R. Denys, I. Yu Zavaliy, Yu Kosarchyn
Summary: MgH2-based nanocomposites were synthesized using reactive ball milling and various catalytic additives. The additives improved the hydrogen absorption-desorption kinetics and stability of the composites. Nano-Ti showed the most stable hydrogen absorption-desorption characteristics compared to TiO2 and Ti4Fe2Ox additives.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Materials Science, Multidisciplinary
Yujie Lv, Bao Zhang, Haixiang Huang, Bogu Liu, Wei Lv, Jianguang Yuan, Guanglin Xia, Xuebin Yu, Dalin Sun, Ying Wu
Summary: Metal borohydride ammoniates have shown promise as hydrogen storage materials, but are hindered by high desorption temperature and ammonia release. By adding NbF5 to Mg(BH4)2·2NH3, lower onset dehydriding temperatures (53-57°C) and higher dehydriding capacities (5.6 wt.%-8.2 wt.%) were achieved with complete suppression of ammonia. The addition of NbF5 also resulted in faster hydrogen release and lower activation energy. Mechanically reacting Mg(BH4)2·2NH3 with NbF5 leads to the formation of dual-metal (Mg, Nb) borohydride ammoniate and MgF2, improving hydrogen diffusion during dehydrogenation.
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Hui Luo, Yunshu Yang, Liwen Lu, Guangxu Li, Xinhua Wang, Xiantun Huang, Xiaoma Tao, Cunke Huang, Zhiqiang Lan, Wenzheng Zhou, Jin Guo, Haizhen Liu
Summary: In this study, a two-dimensional Ti3CN MXene was synthesized and added to the Li-Mg-B-H composite, resulting in a reduction in the dehydrogenation temperature and induction period of the composite. The reversible capacity and capacity retention ratio of the composite were maintained at high levels. Micro-structure studies revealed the transformation of Ti3CN into highly-dispersed nano-TiB2, which acted as an active catalyst to improve the kinetics and reversibility of the composite. This research provides insights into the role of MXene in tailoring the hydrogen storage properties of metal borohydride-based composites.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Lucia Gomez-Coma, Diogo L. Silva, Alfredo Ortiz, Carmen M. Rangel, Victor Manuel Ortiz-Martinez, Alexandra M. F. R. Pinto, Inmaculada Ortiz
Summary: Finding stable solutions for hydrogen storage is crucial for its widespread usage as an energy source and to reduce carbon emissions. This study examines the effects of non-toxic and environmentally friendly additives on the hydrolysis process for releasing hydrogen. Sodium carboxymethyl cellulose and polyacrylamide show promising results as additives for efficient hydrogen production.
APPLIED SCIENCES-BASEL
(2023)
Article
Chemistry, Physical
Noemi Leick, Nicholas A. Strange, Andreas Schneemann, Vitalie Stavila, Karl Gross, Nancy Washton, Amy Settle, Madison B. Martinez, Thomas Gennett, Steven T. Christensen
Summary: This study utilizes nanoencapsulation and chemical additives simultaneously to modify borohydrides by using atomic layer deposition (ALD). The use of trimethylaluminum and water in the ALD process significantly improves the low-temperature H2 capacity and desorption kinetics of magnesium borohydride, while suppressing the release of diborane. These results suggest the potential of ALD as a method to functionalize solid-state H2 storage materials.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Qian Li, Ning Miao, Jinling Zhong, Chengzhang Wu, Haiyan Leng
Summary: This study investigates the effect of KH on the hydrogen storage properties of graphene-doped MgH2, in comparison with KOH. The results demonstrate that the addition of 1 wt% KH and 1 wt% graphene significantly enhances the hydrogen storage performance of MgH2. It desorbs 6.0 wt% H2 within 30 min at 300°C, faster than pure MgH2. However, the desorption rate and activation energy are slower and larger, respectively, than the sample doped with KOH and graphene. Formation of the catalyst KMgH3 is observed with both KH and KOH, indicating that the H-H exchange between KH and MgH2 may suppress the desorption of MgH2, while the in-situ formed MgO by KOH addition promotes MgH2 desorption.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Lili Zhang, Siyu Jin, Mengxue Ren, Cheng Lu, Feng Peng, Gennady L. Gutsev
Summary: The magnesium-lanthanum-hydrogen systems show good stability and high hydrogen storage capacity, providing new insights for the design and synthesis of novel hydrogen storage materials.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Review
Materials Science, Multidisciplinary
Yujie Lv, Ying Wu
Summary: Hydrogen storage in solid-state materials is considered to be a promising technology due to its efficiency, low risk and cost. Mg(BH4)2 is a potential material for hydrogen storage, but research has been done to improve its thermodynamics and kinetics due to its drawbacks.
PROGRESS IN NATURAL SCIENCE-MATERIALS INTERNATIONAL
(2021)
Article
Chemistry, Physical
Nicholas A. Strange, Noemi Leick, Sarah Shulda, Andreas Schneemann, Vitalie Stavila, Andrew S. Lipton, Michael F. Toney, Thomas Gennett, Steven T. Christensen
Summary: Magnesium borohydride is a promising material for hydrogen storage, but its slow dehydrogenation kinetics and formation of intermediate polyboranes limit its application in clean energy technologies. This study presents a novel approach of modifying the physicochemical properties of magnesium borohydride by adding reactive molecules in the vapor phase. The effects of four different molecules on the additive-Mg(BH4)(2) interaction and hydrogen release at lower temperatures are examined. The results demonstrate the efficacy of this approach and provide a new path for additive-based modification of hydrogen storage materials.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Keith G. Ray, Leonard E. Klebano, Vitalie Stavila, ShinYoung Kang, Liwen F. Wan, Sichi Li, Tae Wook Heo, Mark D. Allendorf, Jonathan R. I. Lee, Alexander A. Baker, Brandon C. Wood
Summary: In this study, direct ab initio molecular dynamics simulations were used to investigate the hydrogenation chemistry of MgB2. The research reveals the multistep reaction processes at complex interfaces and provides guidance for improving the kinetic performance of MgB2-based hydrogen storage materials. These findings also serve as a template for exploring chemical pathways in other solid-state energy storage reactions.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Johannes W. M. Osterrieth, Jarnes Rampersad, David Madden, Nakul Rampal, Luka Skoric, Bethany Connolly, Mark D. Allendorf, Vitalie Stavila, Jonathan L. Snider, Rob Ameloot, Joao Marreiros, Conchi Ania, Diana Azevedo, Enrique Vilarrasa-Garcia, Bianca F. Santos, Xian-He Bu, Ze Chang, Hana Bunzen, Neil R. Champness, Sarah L. Griffin, Banglin Chen, Rui-Biao Lin, Benoit Coasne, Seth Cohen, Jessica C. Moreton, Yamil J. Colon, Linjiang Chen, Rob Clowes, Francois-Xavier Coudert, Yong Cui, Bang Hou, Deanna M. D'Alessandro, Patrick W. Doheny, Mircea Dinca, Chenyue Sun, Christian Doonan, Michael Thomas Huxley, Jack D. Evans, Paolo Falcaro, Raffaele Ricco, Omar Farha, Karam B. Idrees, Timur Islamoglu, Pingyun Feng, Huajun Yang, Ross S. Forgan, Dominic Bara, Shuhei Furukawa, Eli Sanchez, Jorge Gascon, Selvedin Telalovic, Sujit K. Ghosh, Soumya Mukherjee, Matthew R. Hill, Muhammed Munir Sadiq, Patricia Horcajada, Pablo Salcedo-Abraira, Katsumi Kaneko, Radovan Kukobat, Jeff Kenvin, Seda Keskin, Susumu Kitagawa, Ken-ichi Otake, Ryan P. Lively, Stephen J. A. DeWitt, Phillip Llewellyn, Bettina Lotsch, Sebastian T. Emmerling, Alexander M. Putz, Carlos Marti-Gastaldo, Natalia M. Padial, Javier Garcia-Martinez, Noemi Linares, Daniel Maspoch, Jose A. Suarez del Pino, Peyman Moghadam, Rama Oktavian, Russel E. Morris, Paul S. Wheatley, Jorge Navarro, Camille Petit, David Danaci, Matthew J. Rosseinsky, Alexandros P. Katsoulidis, Martin Schroder, Xue Han, Sihai Yang, Christian Serre, Georges Mouchaham, David S. Sholl, Raghuram Thyagarajan, Daniel Siderius, Randall Q. Snurr, Rebecca B. Goncalves, Shane Telfer, Seok J. Lee, Valeska P. Ting, Jemma L. Rowlandson, Takashi Uemura, Tomoya Liyuka, Monique A. van derVeen, Davide Rega, Veronique Van Speybroeck, Sven M. J. Rogge, Aran Lamaire, Krista S. Walton, Lukas W. Bingel, Stefan Wuttke, Jacopo Andreo, Omar Yaghi, Bing Zhang, Cafer T. Yavuz, Thien S. Nguyen, Felix Zamora, Carmen Montoro, Hongcai Zhou, Angelo Kirchon, David Fairen-Jimenez
Summary: Porosity and surface area analysis are important in modern materials science. However, there is a lack of attention to the reproducibility issue in calculating BET surface areas from identical isotherms, raising concerns over the reliability of reported BET areas. To address this, a new computational approach called BET surface identification (BETSI) has been developed for accurately and systematically determining the BET area of nanoporous materials.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Chaochao Dun, Sohee Jeong, Deok-Hwang Kwon, ShinYoung Kang, Vitalie Stavila, Zhuolei Zhang, Joo-Won Lee, Tracy M. Mattox, Tae Wook Heo, Brandon C. Wood, Jeffrey J. Urban
Summary: The chemical interactions on the surface of nanoparticles are closely related to its crystal facets, which can regulate the energy storage properties. This study investigated the growth of magnesium particles with different crystal facets on graphene oxide. The hydrogen storage performance of the magnesium particles varied depending on the crystal facet orientation. The results provide a new method for regulating the hydrogen storage of metal hydrides.
CHEMISTRY OF MATERIALS
(2022)
Article
Multidisciplinary Sciences
Luning Chen, Pragya Verma, Kaipeng Hou, Zhiyuan Qi, Shuchen Zhang, Yi-Sheng Liu, Jinghua Guo, Vitalie Stavila, Mark D. Allendorf, Lansun Zheng, Miquel Salmeron, David Prendergast, Gabor A. Somorjai, Ji Su
Summary: Developing highly efficient and reversible hydrogenation-dehydrogenation catalysts is of great importance for hydrogen storage technologies. The authors have developed a highly efficient and reversible single-site platinum catalyst that exhibits excellent catalytic performance in the hydrogenation-dehydrogenation reactions of large molecules such as cyclohexane and methylcyclohexane.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Matthew Green, Katty Kaydanik, Miguel Orozco, Lauren Hanna, Maxwell A. T. Marple, Kimberly Alicia Strange Fessler, Willis B. Jones, Vitalie Stavila, Patrick A. Ward, Joseph A. Teprovich
Summary: This study demonstrates the robust and stable nature of a closo-borate based gel polymer electrolyte (GPE), which enables outstanding electrochemical stability and capacity retention upon extensive cycling. The GPE has a high ionic conductivity and can be used with a lithium metal electrode for extended cycling. It can also be incorporated into a flexible battery.
Article
Chemistry, Physical
Nayely Pineda-Romero, Matthew Witman, Vitalie Stavila, Claudia Zlotea
Summary: We conducted a thorough study on the effect of adding 10% Al into the Ti0.33V0.33Nb0.33 alloy on the hydrogen storage properties. The results showed that while the storage capacity decreased by 20%, several other properties were enhanced by the presence of Al, such as lower hydrogen desorption temperature and improved stability during cycling. This study demonstrates that adding Al into multi-principal element alloys is a promising strategy for designing novel materials for hydrogen storage.
Article
Chemistry, Physical
Helen Correll, Noemi Leick, Rachel E. Mow, Glory A. Russell-Parks, Simon H. Pang, Thomas Gennett, Wade A. Braunecker
Summary: Poly(ethylenimine) (PEI) is an efficient carbon capture medium with high surface area and low volatility when loaded onto mesoporous oxide supports. This study focuses on understanding the influence of nanoconfinement on polymer segmental mobility, which is critical for developing more efficient direct air capture (DAC) systems. A fluorescent probe molecule based on tetrakis(4-hydroxyphenyl)ethylene is developed to indicate the viscosity of the supporting medium, providing insights into polymer dynamics and confinement effects in mesoporous silica.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Inorganic & Nuclear
Joseph E. Reynolds, Austin C. Acosta, ShinYoung Kang, Sichi Li, Andrew S. Lipton, Mark E. Bowden, Nicholas R. Myllenbeck, Andreas Schneemann, Noemi Leick, Austin Bhandarkar, Christopher Reed, Robert D. Horton, Thomas Gennett, Brandon C. Wood, Mark D. Allendorf, Vitalie Stavila
Summary: This study reports a new class of Grignard reagents, reactive borohydride anions replacing halides, which adds a new synthetic dimension and exhibits unique reactivity and potential applications.
Article
Chemistry, Multidisciplinary
Donald A. Robinson, Michael E. Foster, Christopher H. Bennett, Austin Bhandarkar, Elizabeth R. Webster, Aleyna Celebi, Nisa Celebi, Elliot J. Fuller, Vitalie Stavila, Catalin D. Spataru, David S. Ashby, Matthew J. Marinella, Raga Krishnakumar, Mark D. Allendorf, A. Alec Talin
Summary: This report introduces a new material, RuPBA, which has tunable oxidation state and can control artificial synapses through conductivity. Compared to traditional materials, RuPBA has significantly improved retention of programmed states and shows good biocompatibility with neuronal cells, making it a promising candidate for brain-computer interfacing.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Harini Gunda, Keith G. Ray, Leonard E. Klebanoff, Chaochao Dun, Maxwell A. T. Marple, Sichi Li, Peter Sharma, Raymond W. Friddle, Joshua D. Sugar, Jonathan L. Snider, Robert D. Horton, Brendan C. Davis, Jeffery M. Chames, Yi-Sheng Liu, Jinghua Guo, Harris E. Mason, Jeffrey J. Urban, Brandon C. Wood, Mark D. Allendorf, Kabeer Jasuja, Vitalie Stavila
Summary: Metal boride nanostructures have great potential for hydrogen storage applications. However, their synthesis is challenging due to high surface energy, strong bonding, and difficult surface termination. Mechanochemical exfoliation of magnesium diboride in zirconia produces ultrathin MgB2 nanosheets with high yield. High-pressure hydrogenation and dehydrogenation of these nanosheets reveal a hydrogen capacity 50 times larger than bulk MgB2. The enhancement is attributed to defective sites created by ball-milling and incomplete Mg surface coverage. The exfoliation and creation of ultrathin layers offer a promising direction for high-capacity hydrogen storage.
Article
Chemistry, Physical
Suman Chhetri, Anh Tuan Nguyen, Sehwan Song, Nicolas Gaillard, Godwin Severa, Tianwei Ma, Sang-Hee Yoon, Woochul Lee
Summary: Researchers fabricated graphite nanoflake/polydimethylsiloxane nanocomposites with different concentrations, and found that the optimum concentration for maximum solar absorption was 3 wt%. The nanocomposite showed a total solar absorption of 94.8% and was used to develop a floatable interfacial water evaporator with a high evaporation rate and solar-vapor conversion efficiency.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Thi Kieu Ngan Pham, Edward Bruffey, Anh Tuan Nguyen, Ricardo A. Rivera-Maldonado, Ding-Yuan Kuo, Brandi Cossairt, Woochul Lee, Godwin Severa, Joseph J. Brown
Summary: This study successfully synthesized and deposited MgB2 thin films on a gold surface using a wet-chemistry colloid synthesis and deposition process, circumventing the extreme conditions of conventional physical deposition methods. Gas adsorption experiments, X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM) characterization were conducted to validate the functionality and obtain meaningful data of the deposited MgB2 films. A similar synthesis method was applied on an evaporated Au film on glass, and the film thickness was measured to be 3.9 nm using scanning transmission electron microscopy (STEM). AFM roughness measurements confirmed the successful mitigation of the coffee-ring effect.
Article
Chemistry, Physical
Glory A. Russell-Parks, Noemi Leick, Maxwell A. T. Marple, Nicholas A. Strange, Brian G. Trewyn, Simon H. Pang, Wade A. Braunecker
Summary: Direct air capture (DAC) technology is being explored as a pathway for reducing greenhouse gas emissions through efficient removal of CO2 from the atmosphere. However, there is still a knowledge gap in understanding the factors that impact the behavior of these systems in real-world environments. Studying polymer mobility in DAC systems using fluorescence techniques and correlating it with CO2 adsorption kinetics and environmental conditions can provide valuable insights for more efficient operation in real-world conditions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Inorganic & Nuclear
Noemi Leick, Ba L. Tran, Mark E. Bowden, Thomas Gennett, Tom Autrey
Summary: This study investigated the thermal stability of coordination complexes formed between different glymes with Mg(BH4)(2), revealing diverse phase transitions, speciations, and decomposition pathways despite their structural similarities.
DALTON TRANSACTIONS
(2022)