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液体/液体インターフェイスでの酸素減少のメカニズム研究ハイブリッド超微電子と質量スペクトロメトリ

Chaoyue Gu¹, Xin Nie¹, Jiezhang Jiang¹

¹Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering , Peking University , Beijing 100871 , China.

Journal of the American Chemical Society

|July 30, 2019

まとめ

この研究は,液体/液体界面での陽子結合電子移転反応を調査するための新しい電気化学-質量スペクトロメトリー法を導入します. この方法は酸素還元反応における重要な中間物質を成功裏に特定しこれらの重要な化学過程の理解を深めました

科学分野:

電気化学
マススペクトロメトリー
インタフェース科学
カタリシス

背景:

陽子結合電子移転 (PCET) 反応は生物学的および化学的プロセスにおいて不可欠である.
ダイナミックな液体/液体インターフェイスでのPCETメカニズムを調査することは,直接的な中間証拠がないため,困難です.
既存の方法は,間接的な電気化学的およびスペクトル学的データに依存しています.

研究の目的:

液体/液体界面でのPCET反応を研究するための新しい in situ 方法を開発する.
コバルトテトラフェニルポルフィン (CoTPP) によって触媒化された酸素還元反応 (ORR) の主要な中間物質を液体/液体界面で特定する.
ソフトインターフェイスでの反応メカニズムの直接的な証拠を提供する.

主な方法:

新しい電気化学質量スペクトロメトリー (EC-MS) 技術の開発.
二重マイクロ/ナノピペットを用いて凝固した液体/液体のインターフェイスを形成するゲルハイブリッドの超微電子を作ります.
これらの固体化されたインターフェイスを電気化学セルやナノスプレーエミッターとしてマススペクトロメトリーに使用する.

主要な成果:

液体/液体界面での酸素還元反応 (ORR) を研究するためにEC-MS方法を成功裏に適用した.
ORRの主要なコバルトテトラフェニルポルフィン (CoTPP) の中間物質を初めて特定した.
理論的シミュレーションで裏付けられ,4電子の酸素還元経路が優位であることを示した.

結論:

新しいEC-MSプラットフォームは,液体/液体のインターフェイスでの中間物質の現地追跡と識別を可能にします.
この方法は,ORRおよび他の複雑な界面反応のメカニズムに関する貴重な洞察を提供します.
開発されたプラットフォームは,ソフトなインターフェイスでの様々な反応を研究するために有望です.

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