Sustainable reduced graphene oxide (rGO) carbocatalysts for molecular oxygen activation have been developed based on the concept that chemical reduction of graphene oxide to rGO introduces functional groups that can become active sites. Thus, a series of rGOs prepared using hydroquinone (HQ), hydrazine (HZ) and ascorbic acid (ASC) as reducing agents have been tested as catalysts in the aerobic oxidations of thiophenol and indane. In both oxidation reactions, rGO reduced by HQ (rGO-HQ) exhibited the highest catalytic activity and stability. A high selectivity of ol/one (90 %) at around 30 % indane conversion in the absence of transition metals was achieved. Reusability test showed that the activity of rGO-HQ is mostly retained in three consecutive runs. Quenching experiments indicated that the reaction proceeds with the generation of hydroxyl and carbon centered radicals. The higher activity of rGO-HQ was attributed to the covalent anchoring of some HQ molecules on rGO during the chemical reduction. This knowledge has been used to develop a HQ-functionalized Merrifield resin that in spite of its very different textural properties compared to rGO also exhibits catalytic activity for O₂ activation. The present work illustrates the potential to develop rGO carbocatalysts with an increased density of active sites by selecting an appropriate reducing agent during the chemical reduction of graphene oxide.

基于将氧化石墨烯化学还原为rGO引入可以成为活性位点的官能团这一概念，开发了用于分子氧活化的可持续还原氧化石墨烯（rGO）碳催化剂。因此，已经测试了使用对苯二酚（HQ），肼（HZ）和抗坏血酸（ASC）作为还原剂制备的一系列rGO，作为苯硫酚和茚满的好氧氧化中的催化剂。在两个氧化反应中，被HQ还原的rGO（rGO-HQ）表现出最高的催化活性和稳定性。在不存在过渡金属的情况下，在约30％的茚满转化率下实现了ol / one（90％）的高选择性。可重用性测试表明，rGO-HQ的活性在三个连续运行中大部分保留。淬火实验表明，反应随着羟基和碳中心自由基的产生而进行。rGO-HQ的较高活性归因于化学还原过程中某些HQ分子在rGO上的共价锚定。该知识已被用于开发一种HQ官能化的Merrifield树脂，尽管其与rGO相比具有非常不同的质构特性，但对O仍具有催化活性。₂激活。本工作说明了通过在氧化石墨烯的化学还原过程中选择合适的还原剂来开发活性位点密度增加的rGO碳催化剂的潜力。