Template free mild hydrothermal synthesis of core-shell Cu2O(Cu)@CuO visible light photocatalysts for N-acetyl-para-aminophenol degradation
Template free mild hydrothermal synthesis of core-shell Cu2O(Cu)@CuO visible light photocatalysts for N-acetyl-para-aminophenol degradation
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DOI：
10.1039/c9ta07009e
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发表时间：
2019-09-28
影响因子：
11.9
通讯作者：
Wilson, Karen
中科院分区：
文献类型：
--
作者：
Karthikeyan, Sekar;Chuaicham, Chitiphon;Wilson, Karen
太阳能光催化过程是一种很有前途的环境修复方法，但其实施需要改进可见光的收集和转换，并将重点放在低成本、地球资源丰富的材料上。半导体铜氧化物是一种很有前途的可见光催化剂，可用于太阳能燃料和废水净化。本文报道了温和的水热(无模板)合成核壳Cu2O(Cu)@CuO光催化体系，用于可见光催化降解N-乙酰-对氨基苯酚(APAP)。在不同的合成条件下形成了直径在200 nm到2.5 mm之间的中空的、拨浪形的核壳纳米球聚集体；它们都由一个由10-50 nm纳米粒子组成的内部Cu2O外壳组成，周围环绕着CuO纳米粒子的保护性电晕。较高的还原剂和结构导向剂浓度促进了蛋黄状Cu2O/Cu核的形成，伴随着光物理性质的改善，尤其是高的氧化电位和抑制的载流子复合，这与最高的表观量子效率(8%)和APAP的去除速率(7mmolg(-1)min(-1))相关。捕集实验表明，羟基自由基是APAP氧化为苯二酚和短链羧酸的主要活性物种。振荡型核壳结构的Cu2O/Cu@CuO纳米球对APAP光催化降解表现出良好的物理化学稳定性和可回收性。
Solar photocatalytic processes are a promising approach to environmental remediation, however their implementation requires improvements in visible light harvesting and conversion and a focus on low cost, Earth abundant materials. Semiconducting copper oxides are promising visible light photocatalysts for solar fuels and wastewater depollution. Here we report the mild, hydrothermal (template-free) synthesis of core-shell Cu2O(Cu)@CuO photocatalytic architectures for the visible light photocatalytic degradation of N-acetyl-para-aminophenol (APAP). Hollow and rattle-like core-shell nanosphere aggregates with diameters between 200 nm and 2.5 mm formed under different synthesis conditions; all comprised an inner Cu2O shell, formed of 10-50 nm nanoparticles, surrounded by a protective corona of CuO nanoparticles. High reductant and structure-directing agent concentrations promoted the formation of a yolk-like Cu2O/Cu core, associated with improved photophysical properties, notably a high oxidation potential and suppressed charge carrier recombination, that correlated with the highest apparent quantum efficiency (8%) and rate of APAP removal (7 mmol g(-1) min(-1)). Trapping experiments demonstrated hydroxyl radicals were the primary active species responsible for APAP oxidation to quinones and short chain carboxylic acids. Rattle-like core-shell Cu2O/Cu@CuO nanospheres exhibited excellent physiochemical stability and recyclability for APAP photocatalytic degradation.