Abstract：
Regulating the distribution of reactive oxygen species generated from H2 O2 activation is the prerequisite to ensuring the efficient and safe use of H2 O2 in the chemistry and life science fields. Herein, we demonstrate that constructing a dual Cu-Fe site through the self-assembly of single-atomic-layered Cu5 nanoclusters onto a FeS2 surface achieves selective H2 O2 activation with high efficiency. Unlike its unitary Cu or Fe counterpart, the dual Cu-Fe sites residing at the perimeter zone of the Cu5 /FeS2 interface facilitate H2 O2 adsorption and barrierless decomposition into ⋅OH via forming a bridging Cu-O-O-Fe complex. The robust in situ formation of ⋅OH governed by this atomic-layered catalyst enables the effective oxidation of several refractory toxic pollutants across a broad pH range, including alachlor, sulfadimidine, p-nitrobenzoic acid, p-chlorophenol, p-chloronitrobenzene. This work highlights the concept of building a dual catalytic site in manipulating selective H2 O2 activation on the surface molecular level towards efficient environmental control and beyond.
摘要：
调节H2O2活化产生的活性氧的分布是确保H2O2在化学和生命科学领域有效和安全使用的前提。在这里，我们证明了通过单原子层状Cu5纳米团簇在FeS2表面上的自组装来构建双Cu-Fe位点可以高效地实现选择性H2O2活化。与单一的Cu或Fe对应物不同，位于Cu5/FeS2界面周边区域的双Cu-Fe位点通过形成桥接的Cu-O-O-Fe络合物，促进H2O2吸附和无障碍分解为·OH。由这种原子层状催化剂控制的·OH的强大原位形成能够在宽pH范围内有效氧化几种难降解的有毒污染物，包括甲草胺,磺胺嘧啶,对硝基苯甲酸,对氯苯酚,对氯硝基苯.这项工作强调了在表面分子水平上操纵选择性H2O2活化以实现有效的环境控制及以后，建立双重催化位点的概念。
