Graphene-Tailored Thermodynamics and Kinetics to Fabricate Metal Borohydride Nanoparticles with High Purity and Enhanced Reversibility

Hongyu Zhang; Guanglin Xia; Jian Zhang; Dalin Sun; Zaiping Guo; Xuebin Yu

doi:10.1002/aenm.201702975

Graphene-Tailored Thermodynamics and Kinetics to Fabricate Metal Borohydride Nanoparticles with High Purity and Enhanced Reversibility

Hongyu Zhang, Guanglin Xia^*, Jian Zhang, Dalin Sun, Zaiping Guo, Xuebin Yu

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

83 Citations (Scopus)

Abstract

Due to their ultrahigh theoretical capacity, metal borohydrides are considered to be one of the most promising candidate hydrogen storage materials. Their application still suffers, however, from high operating temperature, sluggish kinetics, and poor reversibility. Designing nanostructures is an effective way of addressing these issues, but seeking suitable approaches remains a big challenge. Here, a space-confined solid-gas reaction to synthesize Mg(BH4)2 nanoparticles supported on grapheme is reported, which serves as the structural support for the dispersed Mg(BH4)2 nanoparticles. More notably, density functional theory calculations reveal that graphene could weaken both the MgH bonds of MgH2 and BB bonds of B2H6, which could thermodynamically and kinetically facilitate the chemical transformation to synthesize Mg(BH4)2 with high purity. Because of the synergistic effects of both the significant reduction in particle size and the catalytic effect of graphene, an onset dehydrogenation temperature of ≈154 °C is observed for Mg(BH4)2 nanoparticles, and a complete dehydrogenation could be achieved at a temperature as low as 225 °C, with the formation of MgB2 as the by-product. This work provides a new perspective to tailoring the thermodynamics and kinetics of chemical reactions toward the favorable synthesis of functional inorganic materials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Original language	English
Article number	1702975
Journal	Advanced Energy Materials
Volume	8
Issue number	13
DOIs	https://doi.org/10.1002/aenm.201702975
Publication status	Published - 4 May 2018
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to <a href="mailto:[email protected]">[email protected]</a>.

Funding

This work was partially supported by the National Science Fund for Distinguished Young Scholars (51625102), National Key Research and Development Program of China (2017YFA0204600), the National Natural Science Foundation of China (51471053), the Science and Technology Commission of Shanghai Municipality (17XD1400700), and a Discovery Early Career Researcher Award (DE170100362).

Research Keywords

borohydrides
graphene
hydrogen storage
kinetics
magnesium hydride

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access Output

10.1002/aenm.201702975

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

Cite this

@article{43be8ed559c64e29bb23bba3fc734daf,

title = "Graphene-Tailored Thermodynamics and Kinetics to Fabricate Metal Borohydride Nanoparticles with High Purity and Enhanced Reversibility",

abstract = "Due to their ultrahigh theoretical capacity, metal borohydrides are considered to be one of the most promising candidate hydrogen storage materials. Their application still suffers, however, from high operating temperature, sluggish kinetics, and poor reversibility. Designing nanostructures is an effective way of addressing these issues, but seeking suitable approaches remains a big challenge. Here, a space-confined solid-gas reaction to synthesize Mg(BH4)2 nanoparticles supported on grapheme is reported, which serves as the structural support for the dispersed Mg(BH4)2 nanoparticles. More notably, density functional theory calculations reveal that graphene could weaken both the MgH bonds of MgH2 and BB bonds of B2H6, which could thermodynamically and kinetically facilitate the chemical transformation to synthesize Mg(BH4)2 with high purity. Because of the synergistic effects of both the significant reduction in particle size and the catalytic effect of graphene, an onset dehydrogenation temperature of ≈154 °C is observed for Mg(BH4)2 nanoparticles, and a complete dehydrogenation could be achieved at a temperature as low as 225 °C, with the formation of MgB2 as the by-product. This work provides a new perspective to tailoring the thermodynamics and kinetics of chemical reactions toward the favorable synthesis of functional inorganic materials. {\textcopyright} 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

keywords = "borohydrides, graphene, hydrogen storage, kinetics, magnesium hydride",

author = "Hongyu Zhang and Guanglin Xia and Jian Zhang and Dalin Sun and Zaiping Guo and Xuebin Yu",

note = "Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to <a href={"}mailto:[email protected]{"}>[email protected]</a>.",

year = "2018",

month = may,

day = "4",

doi = "10.1002/aenm.201702975",

language = "English",

volume = "8",

journal = "Advanced Energy Materials",

issn = "1614-6832",

publisher = "John Wiley & Sons",

number = "13",

}

TY - JOUR

T1 - Graphene-Tailored Thermodynamics and Kinetics to Fabricate Metal Borohydride Nanoparticles with High Purity and Enhanced Reversibility

AU - Zhang, Hongyu

AU - Xia, Guanglin

AU - Zhang, Jian

AU - Sun, Dalin

AU - Guo, Zaiping

AU - Yu, Xuebin

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to <a href="mailto:[email protected]">[email protected]</a>.

PY - 2018/5/4

Y1 - 2018/5/4

N2 - Due to their ultrahigh theoretical capacity, metal borohydrides are considered to be one of the most promising candidate hydrogen storage materials. Their application still suffers, however, from high operating temperature, sluggish kinetics, and poor reversibility. Designing nanostructures is an effective way of addressing these issues, but seeking suitable approaches remains a big challenge. Here, a space-confined solid-gas reaction to synthesize Mg(BH4)2 nanoparticles supported on grapheme is reported, which serves as the structural support for the dispersed Mg(BH4)2 nanoparticles. More notably, density functional theory calculations reveal that graphene could weaken both the MgH bonds of MgH2 and BB bonds of B2H6, which could thermodynamically and kinetically facilitate the chemical transformation to synthesize Mg(BH4)2 with high purity. Because of the synergistic effects of both the significant reduction in particle size and the catalytic effect of graphene, an onset dehydrogenation temperature of ≈154 °C is observed for Mg(BH4)2 nanoparticles, and a complete dehydrogenation could be achieved at a temperature as low as 225 °C, with the formation of MgB2 as the by-product. This work provides a new perspective to tailoring the thermodynamics and kinetics of chemical reactions toward the favorable synthesis of functional inorganic materials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

AB - Due to their ultrahigh theoretical capacity, metal borohydrides are considered to be one of the most promising candidate hydrogen storage materials. Their application still suffers, however, from high operating temperature, sluggish kinetics, and poor reversibility. Designing nanostructures is an effective way of addressing these issues, but seeking suitable approaches remains a big challenge. Here, a space-confined solid-gas reaction to synthesize Mg(BH4)2 nanoparticles supported on grapheme is reported, which serves as the structural support for the dispersed Mg(BH4)2 nanoparticles. More notably, density functional theory calculations reveal that graphene could weaken both the MgH bonds of MgH2 and BB bonds of B2H6, which could thermodynamically and kinetically facilitate the chemical transformation to synthesize Mg(BH4)2 with high purity. Because of the synergistic effects of both the significant reduction in particle size and the catalytic effect of graphene, an onset dehydrogenation temperature of ≈154 °C is observed for Mg(BH4)2 nanoparticles, and a complete dehydrogenation could be achieved at a temperature as low as 225 °C, with the formation of MgB2 as the by-product. This work provides a new perspective to tailoring the thermodynamics and kinetics of chemical reactions toward the favorable synthesis of functional inorganic materials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

KW - borohydrides

KW - graphene

KW - hydrogen storage

KW - kinetics

KW - magnesium hydride

UR - http://www.scopus.com/inward/record.url?scp=85040648169&partnerID=8YFLogxK

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85040648169&origin=recordpage

U2 - 10.1002/aenm.201702975

DO - 10.1002/aenm.201702975

M3 - RGC 21 - Publication in refereed journal

SN - 1614-6832

VL - 8

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 13

M1 - 1702975

ER -

Graphene-Tailored Thermodynamics and Kinetics to Fabricate Metal Borohydride Nanoparticles with High Purity and Enhanced Reversibility

Abstract

Bibliographical note

Funding

Research Keywords

UN SDGs

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Cite this