Joint Center for Artificial Photosynthesis, California Institute of Technology , Pasadena California 91125, United States.
ACS Comb Sci. 2014 Feb 10;16(2):47-52. doi: 10.1021/co400151h. Epub 2014 Jan 21.
Combinatorial synthesis and screening for discovery of electrocatalysts has received increasing attention, particularly for energy-related technologies. High-throughput discovery strategies typically employ a fast, reliable initial screening technique that is able to identify active catalyst composition regions. Traditional electrochemical characterization via current-voltage measurements is inherently throughput-limited, as such measurements are most readily performed by serial screening. Parallel screening methods can yield much higher throughput and generally require the use of an indirect measurement of catalytic activity. In a water-splitting reaction, the change of local pH or the presence of oxygen and hydrogen in the solution can be utilized for parallel screening of active electrocatalysts. Previously reported techniques for measuring these signals typically function in a narrow pH range and are not suitable for both strong acidic and basic environments. A simple approach to screen the electrocatalytic activities by imaging the oxygen and hydrogen bubbles produced by the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is reported here. A custom built electrochemical cell was employed to record the bubble evolution during the screening, where the testing materials were subject to desired electrochemical potentials. The transient of the bubble intensity obtained from the screening was quantitatively analyzed to yield a bubble figure of merit (FOM) that represents the reaction rate. Active catalysts in a pseudoternary material library, (Ni-Fe-Co)Ox, which contains 231 unique compositions, were identified in less than one minute using the bubble screening method. An independent, serial screening method on the same material library exhibited excellent agreement with the parallel bubble screening. This general approach is highly parallel and is independent of solution pH.
组合合成和筛选在发现电催化剂方面受到了越来越多的关注,特别是对于与能源相关的技术。高通量发现策略通常采用快速、可靠的初始筛选技术,该技术能够识别出具有活性的催化剂组成区域。传统的通过电流-电压测量的电化学特性分析在本质上受到吞吐量的限制,因为这种测量最容易通过串行筛选来进行。并行筛选方法可以获得更高的吞吐量,并且通常需要使用催化活性的间接测量。在水分解反应中,可以利用溶液中局部 pH 值的变化或氧气和氢气的存在来进行活性电催化剂的并行筛选。以前报道的用于测量这些信号的技术通常在较窄的 pH 范围内起作用,并且不适合强酸性和碱性环境。这里报道了一种通过成像析氧反应 (OER) 和析氢反应 (HER) 产生的氧气和氢气气泡来筛选电催化活性的简单方法。使用定制的电化学电池记录筛选过程中的气泡演化,其中测试材料经受所需的电化学电势。从筛选中获得的气泡强度瞬变进行定量分析,得到代表反应速率的气泡优值 (FOM)。使用气泡筛选方法在不到一分钟的时间内,从包含 231 种独特成分的赝三元材料库 (Ni-Fe-Co)Ox 中鉴定出了活性催化剂。对同一材料库进行的独立、串行筛选方法与并行气泡筛选具有极好的一致性。这种通用方法具有高度并行性,并且与溶液 pH 无关。