Department of Civil and Environmental Engineering, ‡Department of Materials Science and Engineering, §Department of Engineering and Public Policy, and ∥The Scott Institute for Energy Innovation, Carnegie Mellon University , 5000 Forbes Ave, Pittsburgh, Pennsylvania 15213, United States.
Langmuir. 2017 Nov 7;33(44):12580-12591. doi: 10.1021/acs.langmuir.7b02861. Epub 2017 Oct 26.
We evaluate the efficiency and capacity of electrochemically reversible insertion electrodes for use in targeted ion removal applications in aqueous solutions. The relative attributes of insertion material chemistry are evaluated by comparing the performance of two different sodium insertion materials, NaTi(PO) and NaMnO, in different electrolyte environments. We performed experiments over a range of solution compositions containing both sodium and other non-inserting ions, and we then developed mechanistic insight into the effects of solution concentration and composition on overpotential losses and round trip Coulombic efficiency. In dilute aqueous streams, performance was limited by the rate of ion transport from the bulk electrolyte region to the electrode interface. This leads to slow rates of ion removal, large overpotentials for ion insertion, parasitic charge loss due to water electrolysis, and lower round trip Coulombic efficiencies. This effect is particularly large for insertion electrodes with redox potentials exceeding the water stability window. In solutions with high background concentrations of non-inserting ions, the accumulation of non-inserting ions at the electrode interface limits inserting ion flux and leads to low ion removal capacity and round trip Coulombic efficiency.
我们评估了电化学可逆插入电极在水溶液中用于靶向离子去除应用的效率和容量。通过比较两种不同的钠离子插入材料 NaTi(PO)和 NaMnO 在不同电解质环境下的性能,评估了插入材料化学性质的相对属性。我们在含有钠和其他非插入离子的一系列溶液组成范围内进行了实验,然后深入了解了溶液浓度和组成对过电势损失和往返库仑效率的影响。在稀水溶液中,性能受到从主体电解质区域到电极界面的离子传输速率的限制。这导致离子去除速率较慢,离子插入的过电势较大,由于水电解而产生寄生电荷损失,以及往返库仑效率较低。对于氧化还原电位超过水稳定窗口的插入电极,这种影响特别大。在具有高背景浓度非插入离子的溶液中,非插入离子在电极界面处的积累限制了插入离子的通量,导致离子去除容量和往返库仑效率低。