醋酸盐结合的钴氧化物水氧化催化剂：一价阴离子和阳离子在降低过电位中的作用
An Acetate Bound Cobalt Oxide Catalyst for Water Oxidation: Role of Monovalent Anions and Cations In Lowering Overpotential
摘要：
Co（II）溶于pH 7的乙酸盐缓冲液中，由于其溶解度较高，在相同条件下的水氧化电流明显大于Co（II）溶于磷酸盐缓冲液中的水氧化电流，是一种良好的水氧化催化剂。当电沉积在ITO/FTO电极上时，其形成乙酸盐结合的基于钴（II）氧化物的材料（Co-Ac-WOC），其在pH 7缓冲溶液中在830 mV下显示出0.1 mA/cm $^{2}$的催化水氧化电流密度和在1 V下显示出1 mA/cm $^{2}$的催化水氧化电流密度。用AFM、HR-TEM和SEM（在不同时间和电沉积电位下）研究了Co-Ac-OEC的形貌。利用XPS、EDX、燃烧分析和ATR-FTIR研究了Co-Ac-OEC的化学组成，表明该材料具有CoO核，并且氯离子和乙酸根阴离子结合到Co中心。发现钠被整合在Co-Ac-WOC中。钠离子和氯离子的存在使析氧反应（OER）的起始电位相对于pH 7下的经典Co-Pi降低240 mV。较低的起始电位和较高的OER电流使Co-Ac-WOC中的交换电流密度降低至10 $^{-6.7}$，相对于Co-Pi及其衍生物中的10 $^{-8}$-10 $^{-10}$。
英文摘要：
Co(II) dissolved in acetate buffer at pH 7 is found to be a good water oxidation catalyst (WOC) showing electrocatalytic water oxidation current significantly greater than Co(II) in phosphate buffer under the same conditions owing to the higher solubility of the former. When electrodeposited on ITO/FTO electrodes it forms acetate bound cobalt(II)oxide based material (Co-Ac-WOC) showing catalytic water oxidation current density of 0.1 mA/cm$^{2}$ at 830 mV and 1 mA/cm$^{2}$ at 1 V in a pH 7 buffer solution. The morphology of Co-Ac-OEC is investigated with AFM, HR-TEM and SEM (at different times and electrodeposition potentials). The chemical composition of Co-Ac-OEC is investigated using XPS, EDX, combustion analysis and ATR-FTIR which indicates that this material has a CoO core with chloride and acetate anions bound to the Co center. Sodium is found to be integrated in the Co-Ac-WOC. The presence of the sodium ions and the chloride ions lowers the onset potential for oxygen evolution reaction (OER) by 240 mV relative to the classic Co-Pi at pH 7. The lower onset potential and higher OER current lowers the exchange current density to 10$^{-6.7}$ in Co-Ac-WOC relative to 10$^{-8}$-10$^{-10}$ in Co-Pi and its derivatives.
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