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首页> 外文期刊>Chemistry: A European journal >Chemoselective Phototransformation of C-H Bonds on a Polymer Surface through a Photoinduced Cerium Recycling Redox Reaction
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Chemoselective Phototransformation of C-H Bonds on a Polymer Surface through a Photoinduced Cerium Recycling Redox Reaction

机译：通过光诱导的铈循环氧化还原反应对聚合物表面的C-H键进行化学选择性光转化

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摘要

It is generally accepted that Ce~(4+) is unable to directly oxidize unreactive alkyl C-H bonds without the assistance of adjacent polar groups. Herein, we demonstrate in our newly developed confined photochemical reaction system that this recognized issue may be challenged. As we found, when a thin layer of a CeCl_3/HCl aqueous solution was applied to a polymeric substrate and the substrate subjected to UV irradiation, Ce~(3+) was first photooxidized to form Ce~(4+) in the presence of H~+, and the in situ formed Ce~(4+) then performs an oxidation reaction on the C-H bonds of the polymer surface to form surface-carbon radicals for radical graft polymerization reactions and functional-group transformations, while reducing to Ce~(3+) and releasing H~+ in the process. This photoinduced cerium recycling redox (PCRR) reaction behaved as a biomimetic system in an artificial recycling reaction, leading to a sustainable chemical modification strategy for directly transforming alkyl C-H bonds on polymer surfaces into small-molecule groups and polymer brushes. This method is expected to provide a green and economical tool for industrial applications of polymer-surface modification.
机译：人们普遍认为，Ce〜（4+）在没有相邻极性基团的帮助下不能直接氧化未反应的烷基C-H键。在此，我们在我们最新开发的密闭光化学反应系统中证明了这一公认的问题可能会受到挑战。正如我们发现的那样，当将CeCl_3 / HCl水溶液的薄层施加到聚合物基材上并对该基材进行UV辐照时，首先在有NaCl的存在下将Ce〜（3+）光氧化形成Ce〜（4+）。 H〜+，然后原位形成的Ce〜（4+）在聚合物表面的CH键上进行氧化反应，形成表面碳自由基，用于自由基接枝聚合反应和官能团转化，同时还原为Ce〜 （3+），然后释放H〜+。这种光致诱导的铈循环氧化还原（PCRR）反应在人工循环反应中表现为仿生系统，从而导致了可持续的化学修饰策略，可将聚合物表面的烷基C-H键直接转化为小分子基团和聚合物刷。该方法有望为聚合物表面改性的工业应用提供一种绿色经济的工具。

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