Pseudocapacitive Energy Storage and Electrocatalytic Hydrogen- Evolution Activity of Defect-Ordered Perovskites SrxCa3-xGaMn2O8 (x=0 and 1)

被引:34
|
作者
Karki, Surendra B. [1 ]
Ramezanipour, Farshid [1 ]
机构
[1] Univ Louisville, Dept Chem, Louisville, KY 40292 USA
基金
美国国家科学基金会;
关键词
pseudocapacitor; hydrogen-evolution reaction; oxide; ordering; stability;
D O I
10.1021/acsaem.0c01935
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The diverse range of possible arrangements of oxygen vacancies in oxygen-deficient perovskites results in a variety of structure types and fascinating electrochemical properties. Here, we report Ca3GaMn2O8 and SrCa2GaMn2O8, where the ordering of oxygen vacancies leads to cation and polyhedral order, resulting in a remarkable array of electrochemical properties coexisting in the same compound. Neutron and X-ray diffraction have been utilized to study the structure of these materials that feature simultaneous defect order and cation order. Remarkably, both materials show very high electrocatalytic activity for hydrogen-evolution reaction (HER) of water splitting in bulk form, without the need for composite formation or nanofabrication. The HER overpotential required to achieve a current density of 10 mA/cm(2) is as low as eta(10) approximate to 315 mV. In addition, detailed pseudocapacitive studies show that both compounds are capable of energy storage as anion-based pseudocapacitors, arising from oxygen ion intercalation. The symmetric pseudocapacitor cells fabricated based on these materials show a combination of high energy density and power density. These pseudocapacitor cells are also extremely stable, maintaining their high activity over 1000 cycles of charge-discharge. Electrical charge-transport studies indicate that these compounds have semiconducting properties in a wide temperature range, 25800 degrees C. Magnetic studies using both magnetometry and neutron scattering indicate a transition to an antiferromagnetic state, with a G-type arrangement of spins, where the moment on each Mn is aligned antiparallel to all nearest neighbors. This combination of properties indicates the great potential of this class of defect-ordered systems and their importance to energy research.
引用
收藏
页码:10983 / 10992
页数:10
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