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Solar-to-hydrogen peroxide energy conversion on resorcinol–formaldehyde resin photocatalysts prepared by acid-catalysed polycondensation
Communications Chemistry ( IF 5.9 ) Pub Date : 2020-11-13 , DOI: 10.1038/s42004-020-00421-x
Yasuhiro Shiraishi 1 , Takumi Hagi 1 , Masako Matsumoto 1 , Shunsuke Tanaka 2 , Satoshi Ichikawa 3 , Takayuki Hirai 1
Affiliation  

The photocatalytic generation of hydrogen peroxide from water and dioxygen (H2O + 1/2O2 → H2O2, ΔG° = +117 kJ mol–1) under sunlight is a promising strategy for the artificial photosynthesis of a liquid fuel. We had previously found that resorcinol–formaldehyde (RF) resin powders prepared by the base-catalysed high-temperature hydrothermal method act as semiconductor photocatalysts for H2O2 generation. Herein, we report that RF resins prepared by the acid-catalysed high-temperature hydrothermal method (~523 K) using common acids at pH < 4 exhibit enhanced photocatalytic activity. The base- and acid-catalysed methods both produce methylene- and methine-bridged resins consisting of π-conjugated and π-stacked benzenoid–quinoid donor–acceptor resorcinol units. The acidic conditions result in the resins with a lower bandgap (1.7 eV) and higher conductivity because the lower-degree of crosslinking creates a strongly π-stacked architecture. The irradiation of the RF-acid resins with simulated sunlight in water with atmospheric-pressure O2 generates H2O2 at a solar-to-chemical conversion efficiency of 0.7%, which is the highest efficiency ever reported for powder catalysts used in artificial photosynthesis.



中文翻译:

酸催化缩聚制备间苯二酚-甲醛树脂光催化剂的太阳能-过氧化氢能量转化

在阳光下从水和分子氧 (H 2 O + 1/2O 2  → H 2 O 2 , Δ G ° = +117 kJ mol –1 )光催化产生过氧化氢是一种很有前途的液体燃料人工光合作用策略. 我们之前发现碱催化高温水热法制备的间苯二酚-甲醛(RF)树脂粉末可作为H 2 O 2的半导体光催化剂。一代。在此,我们报道了在 pH < 4 下使用普通酸通过酸催化高温水热法 (~523 K) 制备的 RF 树脂表现出增强的光催化活性。碱催化和酸催化方法均产生由 π 共轭和 π 堆叠的苯系物-醌型供体-受体间苯二酚单元组成的亚甲基和次甲基桥接树脂。酸性条件导致树脂具有较低的带隙 (1.7 eV) 和较高的电导率,因为较低的交联度会产生强烈的 π 堆叠结构。射频酸树脂在常压O 2水中模拟阳光照射产生H 2 O 2太阳能到化学的转化效率为 0.7%,这是迄今为止报道的用于人工光合作用的粉末催化剂的最高效率。

更新日期:2020-11-13
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