Hydrogen evolution from organic “hydrides”

Schwarz, Daniel E.; Cameron, Thomas M.; Hay, P. Jeffrey; Scott, Brian L.; Tumas, William; Thorn, David L.

doi:10.1039/b511884k

Cited by 82 publications

(51 citation statements)

References 32 publications

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“…[62] It was found that certain derivatives exhibited exothermic and rapid hydrogen release when reacted with protic acids in the presence of a catalyst. However, these materials were limited to <2 wt pct hydrogen, and so the CHSCoE moved on to other more promising compounds.…”

Section: A Exothermic Hydrocarbons As Chemical Hydrogen Storage Matementioning

confidence: 99%

Accelerating the Understanding and Development of Hydrogen Storage Materials: A Review of the Five-Year Efforts of the Three DOE Hydrogen Storage Materials Centers of Excellence

Klebanoff

Ott

Simpson

et al. 2014

Metallurgical and Materials Transactions E

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A technical review of the progress achieved in hydrogen storage materials development through the U.S. Department of Energy's (DOE) Fuel Cell Technologies Office and the three Hydrogen Storage Materials Centers of Excellence (CoEs), which ran from 2005 to 2010 is presented. The three CoEs were created to develop reversible metal hydrides, chemical hydrogen storage materials, and high-specific-surface-area (SSA) hydrogen sorbents. For each CoE, the approach taken is specified, key outcomes and accomplishments identified, and recommendations for future work are suggested. The Metal Hydride Center of Excellence addresses work on destabilized hydrides, including the LiBH/Mg 2 NiH 4 system, borohydrides, amides, and alanes; and compares the best materials to DOE targets. The Chemical Hydrogen Storage Center of Excellence discusses the classes of materials studied for chemical hydrogen storage, focusing on ammonia borane and examines the progress in developing efficient regeneration schemes. The Hydrogen Sorption Center of Excellence describes the progress in developing high-SSA sorbents and pathways for developing improved materials capable of achieving DOE targets. The phenomenon of spillover is also observed and its importance to ensuring improved measurements is discussed. Through the five-year effort of the Hydrogen Storage Materials Centers of Excellence, significant progress was achieved in developing and understanding hydrogen storage materials.

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Section: A Exothermic Hydrocarbons As Chemical Hydrogen Storage Matementioning

confidence: 99%

Accelerating the Understanding and Development of Hydrogen Storage Materials: A Review of the Five-Year Efforts of the Three DOE Hydrogen Storage Materials Centers of Excellence

Klebanoff

Ott

Simpson

et al. 2014

Metallurgical and Materials Transactions E

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“…The imidazolines were designed to have favorable thermodynamics of hydrogen release by 1,2-elimination dehydrogenation. This was demonstrated by both experiment and theory 3 . The molecules used had large substituents on the imidazolines, which limited the gravimetric storage density to about 1 wt%.…”

Section: Current Statusmentioning

confidence: 76%

“…However, the co product B(O-t-Bu) 3 contains strong B-O bonds and its reduction to AB is prohibitively endothermic (ca. 28 kcal/mol).…”

Section: Spent Fuel Regenerationmentioning

confidence: 99%

“…Currently, each of the Center's three AB regeneration processes consists of four key steps that include digestion of spent fuel BNH x followed by addition of hydride by a reducing agent to form BH 3 units, and addition of ammonia to complete the formation of AB. In addition, the reducing agent also needs to be recycled from MX to MH to complete the AB regeneration cycle.…”

Section: Executive Summarymentioning

confidence: 99%

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Down Select Report of Chemical Hydrogen Storage Materials, Catalysts, and Spent Fuel Regeneration Processes

Ott¹,

Linehan²,

Lipiecki³

et al. 2008

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AcknowledgementsThe authors of this report wish to thank all of the partners of the Chemical Hydrogen Storage Center of Excellence. Without their dedication, technical contributions and teamwork, and the hard work of the students and postdocs involved in this work, this Center would not have been able to accomplish such a significant amount in such a short time. The Center would like to give special thanks to Grace Ordaz (DOE) and Dr. Sunita Satyapal (DOE), for their contributions to the success of our Center, and in the critical reading of the draft report.The CHSCoE was competitively awarded and funded by DOE' Executive SummaryThe Chemical Hydrogen Storage Center of Excellence (CHSCoE) partners have studied more than 60 materials since the Center's inception in early calendar year 2005. This report contains the outcome of the Center's storage material down select process and the status of these materials in moving forward to Phase II R&D conducted by the Center's partners.During the first three years of the Center's research, several concepts for the storage of hydrogen in chemical hydrogen storage materials have been developed and tested. The key classes of materials investigated include endothermic release materials (such as organocarbenes, imidazolines, magnesium alkoxides, and silicon nanoparticles and clathrates), exothermic release materials (such as ammonia borane (AB) and mixtures with ionic liquids or scaffolds containing ammonia borane, metal amidoboranes, and amine boranes), and polyhedral boranes (such as alkali metal salts of decaborane, undecaborane, and dodecaborane anions). To release hydrogen from these classes of materials, approaches including thermolysis, hydrolysis, and catalysis have been or are being developed. All three of these approaches are yielding promising hydrogen storage capacities or rates of hydrogen release or both in some cases. Other concepts (e.g. coupled endothermic/exothermic reactions, nanoparticle hydrides, and polyhedral borane hydrolysis) have also been tested but have not resulted in hydrogen release rates or capacities that have the potential to meet DOE targets for 2010, and these systems have been discontinued for further study.Of the more than 60 materials the CHSCoE investigated, approximately 50% of the materials have been discontinued. They include endothermic imidazolines, nanoparticles and silicon clathrates, magnesium alkoxides, and polyhedral boranes. Certain release concepts of other materials have also been discontinued, such as the use of Bronsted acid catalysis of hydrogen release from ammonia borane, substoichiometric LiH/ammonia borane mixtures, and methylamine borane. Studies of these materials or release concepts are discontinued for reasons of either low capacity, poor release kinetics, high release temperatures, or the spent fuel products require regeneration of borates (regeneration of borates was discontinued as a part of DOE's sodium borohydride go/no go decision at the end of fiscal year 2007).About 30% of the materials show promising capa...

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“…While considerable challenges exist in hydrogen economy, enormous efforts have been focused on developing viable hydrogen storage materials [1]. Previous studies have been devoted to complex light metal hydrides [2] as well as carbon [3][4][5][6][7][8] or BN [9,10] based nanostructures, metal-organic frameworks (MOF) [11][12][13][14][15][16], covalent organic frameworks (COF) [17][18][19][20][21], zeolites [22][23][24], and even organic chemical hydrides [25][26][27][28]. Although many of them exhibit interesting characteristics, the problems still remain due to that they all have poor thermodynamics or kinetics, and actually none in experiment yet meet the new 2017 US Department of Energy target of 5.5 wt% reversible hydrogen storage at ambient condition.…”

Section: Introductionmentioning

confidence: 99%

First-Principles Investigation of Li<sup>+</sup>-Doped Conjugated Microporous Polymer as a Potential Hydrogen Storage Medium

Lu¹

2013

CICC

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Abstract:We used first-principles calculations to investigate the adsorptive binding of hydrogen molecule with lithium doped triethynylbenzene. The prior binding site of Li + is above the C≡C triple bond rather than the aromatic ring at the computational level of UM06-L/6-311G(d,p), which could provide an accurate description of cation-π interaction. For single, double, and multiple dihydrogen interaction with a formula unit of Li + -doped triethynylbenzene, the average binding energies per H2 are found to be in the range of -5.08 ~ -4.58 kcal/mol. The strong binding affinity is promising for hydrogen storage, since it will play a crucial role in physisorption at ambient condition.Further, with a saturated 4-5-5 adsorption, a reversible hydrogen storage capacity of 14.0 wt% is attained. Based on the calculated results, we designed Li cation doped conjugated microporous polymer as hydrogen storage medium and obtained excellent hydrogen uptake performance.

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Hydrogen evolution from organic “hydrides”

Abstract: Benzimidazolines (dihydrobenzimidazoles) are shown for the first time to eliminate hydrogen (H2) by catalyzed reaction with protic compounds.

Cited by 82 publications

References 32 publications

Accelerating the Understanding and Development of Hydrogen Storage Materials: A Review of the Five-Year Efforts of the Three DOE Hydrogen Storage Materials Centers of Excellence

Accelerating the Understanding and Development of Hydrogen Storage Materials: A Review of the Five-Year Efforts of the Three DOE Hydrogen Storage Materials Centers of Excellence

Down Select Report of Chemical Hydrogen Storage Materials, Catalysts, and Spent Fuel Regeneration Processes

First-Principles Investigation of Li<sup>+</sup>-Doped Conjugated Microporous Polymer as a Potential Hydrogen Storage Medium

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