Solid-State Hydroxide Ion Conductivity in Silver(I) Oxide, Ag2O

被引:0
作者
Schulte, Leanna [1 ]
Qin, Shihan [1 ]
Jung, Wonil [1 ]
George, Christy [2 ]
Dillenburger, Jarrett D. [1 ]
Venkatesh, Akshay [1 ]
Ishak, Muhammad K. [3 ]
Wonderling, Nichole M. [3 ]
Marth, Sariah [4 ]
Park, Heemin [4 ]
Bae, Chulsung [4 ]
Rappe, Andrew M. [1 ]
Mallouk, Thomas E. [1 ,5 ]
机构
[1] Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
[2] Penn State Univ, Dept Chem, University Pk, PA 16802 USA
[3] Penn State Univ, Mat Res Inst, University Pk, PA 16802 USA
[4] Rensselaer Polytech Inst, Dept Chem & Chem Biol, Troy, NY 12180 USA
[5] Natl Inst Mat Sci NIMS, Int Ctr Mat Nanoarchitecton WPI MANA, Tsukuba, Ibaraki 3050044, Japan
基金
美国国家科学基金会;
关键词
TOTAL-ENERGY CALCULATIONS; INITIO; ENHANCEMENT;
D O I
10.1021/acs.chemmater.4c02082
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
Silver(I) oxide, Ag2O, precipitated as microcrystals by combining aqueous silver(I) nitrate and KOH solutions, was found to be a solid-state hydroxide ion conductor with ionic conductivity on the order of 10-3 S/cm. The proton chemical shifts at 4.87 and -7.35 ppm measured by solid-state 1H NMR experiments are attributed to water molecules and in-lattice OH- coordinated to silver, respectively. The lack of spinning sidebands around the 4.87 ppm peak indicates rapid reorientation on the NMR time scale, suggesting that the water molecules are adsorbed to the surface of the Ag2O crystals. Pulsed field gradient measurements gave similar diffusion coefficients (2 x 10-7 cm2/s at 298 K) for all three proton environments, indicating chemical exchange between sites on the millisecond time scale. The activation energy for OH- diffusion measured by NMR (0.18 eV) was comparable to that obtained by conductivity measurements and density functional theory (DFT) electronic structure calculations. The calculated Pourbaix diagram of Ag2O is consistent with the slightly lower sample density observed in He pycnometry and thermogravimetric measurements.
引用
收藏
页码:11440 / 11448
页数:9
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