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化学进展 2021, Vol. 33 Issue (9): 1586-1597 DOI: 10.7536/PC200831 前一篇   后一篇

• 综述 •

LiBH4储氢热力学和动力学调控

丁朝1,2, 杨维结3,*(), 霍开富1,*(), Leon Shaw2   

  1. 1 耐火材料与冶金国家重点实验室 先进材料与纳米技术研究院 武汉科技大学 武汉 430081
    2 伊利诺伊理工大学机械、材料和航空航天学院 芝加哥 60616
    3 华北电力大学能源动力与机械工程学院 保定 071003
  • 收稿日期:2020-08-12 修回日期:2020-12-07 出版日期:2021-09-20 发布日期:2020-12-28
  • 通讯作者: 杨维结, 霍开富
  • 基金资助:
    美国国家自然科学基金项目(CMMI-1261782)
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Thermodynamics and Kinetics Tuning of LiBH4 for Hydrogen Storage

Zhao Ding1,2, Weijie Yang3(), Kaifu Huo1(), Leon Shaw2   

  1. 1 The State Key Laboratory of Refractories and Metallurgy, Institute of Advanced Materials and Nanotechnology, Wuhan University of Science and Technology,Wuhan 430081, China
    2 Department of Mechanical, Materials and Aerospace Engineering, Illinois Institute of Technology, Chicago 60616,U.S.A.
    3 School of Energy, Power and Mechanical Engineering, North China Electric Power University, Baoding 071003, China
  • Received:2020-08-12 Revised:2020-12-07 Online:2021-09-20 Published:2020-12-28
  • Contact: Weijie Yang, Kaifu Huo
  • Supported by:
    U.S. National Science Foundation(CMMI-1261782)

为应对能源短缺和气候变化的挑战,调整以化石能源为主的传统能源框架,形成以可再生能源为基础的新型能源结构是我国能源结构升级的必然之路。氢能以其能量密度高、热值大、资源丰富、无污染等优点备受关注。LiBH4作为最有希望的车载固体储氢能源载体之一已有多年研究,但该材料当前仍无法满足工业应用需求。本文围绕LiBH4放/充氢反应稳定的热力学与缓慢的动力学的调控,讨论了当前各种主流工艺及其最新研究成果,包括机械球磨激活、纳米限域、催化剂掺杂改性、离子替代、反应物失稳和高能球磨结合气溶胶喷涂(BMAS)新工艺,旨在为其推广应用提供参考和解决方案。值得注意的是,BMAS有能力帮助LiBH4 + MgH2复合物等热力学有利体系克服其动力学障碍,并在较低温度下提供促进释放氢气的热力学驱动力。

关键词： 储氢材料, LiBH4, 纳米工程, 热力学优化, 动力学改善, 高能球磨结合气溶胶喷涂

To meet the challenge of energy shortage and climate change, it is required to build the new renewable energy based structure and gradually abandon the conventional fossil fuel based energy structure. Hydrogen energy has attracted more and more attention, due to its high energy density, large calorific value, abundant resource and zero pollution. LiBH4, which has been acknowledged as one of the most promising hydrogen storage alternatives for onboard energy carrier applications, is still not qualified for the industrialization, though it has been studied for years. Herein, a state-of-the-art review on the modification of stable thermodynamics and sluggish kinetics of hydrogen storage in LiBH4, aiming to providing reference and solutions for its promotion and application. Multiple main-stream techniques along with their latest efforts have been discussed, including mechanical milling activation, nanoscaffold confinement, catalyst modification, ions substitution, reactant destabilization and a novel process termed as high-energy ball milling with in-situ aerosol spraying (BMAS). Remarkable, BMAS is the technology of proven ability to overcome the kinetic barriers for thermodynamically favorable systems like LiBH4 + MgH2 mixture and provide thermodynamic driving force to enhance hydrogen release at a lower temperature.

Contents

Contents

1 Introduction

2 Thermodynamical tuning of LiBH4

2.1 Cation/anion substitution

2.2 Reactant destabilization

3 Kinetics tuning of LiBH4

3.1 Mechanical milling activation

3.2 Nanoscaffold confinement by the infiltration approach

3.3 Modification by doping catalysts

4 Dual-tuning thermodynamics and kinetics of LiBH4

5 Conclusion and outlook

Key words: hydrogen storage materials, LiBH4, nanoengineering, thermodynamical tuning, kinetics tuning, BMAS
()
图1 (a)LiZn2(BH4)5和(b)NaZn(BH4)3的晶体结构[15]。其中,蓝球、棕球、深灰球和浅灰球分别代表Zn原子、B原子、M(M=Li或Na)原子和H原子
Fig. 1 Crystal structures of (a) LiZn2(BH4)5 and (b) NaZn(BH4)3[15]. Zn blue, B brown, M dark gray (M=Li, Na), H light gray
图2 (a) LiM(BH4)3Cl的晶体结构;(b)一个拥有扭曲M4Cl4立方烷结构的[M4Cl4(BH4)12]4-四核阴离子簇, M=La、Gd[20]
Fig.2 (a) Crystal structure of the novel compounds LiLa(BH4)3Cl and LiGd(BH4)3Cl (b) Isolated tetranuclear anionic clusters [M4Cl4(BH4)12]4- (M = La or Gd) with a distorted cubane M4Cl4 core[20]
图3 LiBH4、MgH2以及LiBH4/MgH2体系的焓变示意图[7]
Fig.3 Enthalpy diagram of LiBH4, MgH2 and LiBH4/MgH2 system[7]
图4 (a)介孔碳空心球(MCHSs)的制备过程示意图,以及MCHSs的(b)SEM图和(c)TEM图[64]
Fig.4 (a) Schematic illustration of the fabrication procedure of MCHSs, (b) SEM and (c) TEM images[64]
图5 SiB4催化LiBH4的脱氢和再吸氢机理示意图[68]
Fig.5 Schematic illustration of dehydrogenation and rehydrogenation mechanism of SiB4 catalyzed LiBH4[68] (b)
图6 LiBH4-0.04(Li3BO3+NbH)体系和块状LiBH4在不同温度下的(a)等温放氢曲线与(b)等温充氢曲线[73]
Fig.6 (a) Isothermal dehydrogenation and (b) hydrogenation curves of the LiBH4-0.04(Li3BO3 + NbH) system and the pristine LiBH4 at different temperatures[73]
图7 (a)全自动BMAS装置设备简图及(b)工作流程图,其中1表示开,0表示关[77]
Fig. 7 (a) Schematic of the automated BMAS device and (b) its operation flow-chart where “1” means “on” and “0” means “off” on the Y axis[77]
图8 LiBH4/THF气溶胶中的LiBH4颗粒的(a)总体和(b)局部放大SEM图[78]
Fig.8 SEM images of LiBH4 particles generated via aerosol spraying of the LiBH4/THF solution using the TSI aerosol generator. (a) A general view and (b) a closer view[78]
图9 (a)BMAS粉末和(b)六次放/充氢循环后粉末的FESEM影像,以及(c)BMAS粉末在不同温度下的放/充氢循环(1~6)曲线[77]
Fig.9 FESEM images of (a) BMAS sample and (b) 6R sample; (c) Comparisons of dehydrogenation and re-hydrogenation behaviors of the BMAS mixtures for six cycles[77]
图10 (a)265 ℃时,BMAS粉末和未处理的MgH2粉末、LiBH4粉末的分解压比较;(b)BMAS粉末与未处理的LiBH4粉末、球磨MgH2粉末的表观活化能比较[94]
Fig.10 (a) The dissociation pressure for BMAS sample at 265 ℃ in comparison with the dissociation pressure of bulk MgH2 and LiBH4; (b) Kissinger plots of the bulk LiBH4, ball-milled MgH2+C, and BMAS powder with 50% LiBH4[94]
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摘要

LiBH4储氢热力学和动力学调控