研究团队报告了一种基于矿物的氧源，而不仅仅是水的实验。该机制涉及在各种地球动力学过程(例如水流和地震)中磨损的矿物-水界面上产生陆地活性氧，这些过程是活跃的，其中自由电子通过开壳电子和点缺陷、高压、水/冰相互作用以及这些过程的组合产生的。本文报道的实验表明，石英或硅酸盐矿物可以产生活性含氧位点(≡SiO·，≡SiOO·)，这些位点最初出现在硅酸盐中的Si-O键的裂解过程中，并在与水接触时产生陆地活性氧。同位素标记的实验表明，过氧自由基的羟基化(≡SiOO·)是H2O2生成的主要途径。这种异构的陆地活性氧生成化学过程，允许氧原子在水和岩石之间转移，并改变它们的同位素组成。
这一过程可能在自然环境中普遍存在，以矿物为基础的H2O2生产和伴随的O2可能发生在地球上，也可能发生在其他类地行星上，提供初始氧化剂和游离氧，并成为生命进化和行星宜居性的一个组成部分。
据介绍，陆地活性氧(ROS)可能在缺氧环境的形成和早期生命的进化中发挥了核心作用。人们对太古代地球上陆地活性氧的非生物起源进行了大量研究，通常认为陆地活性氧起源于H2O/CO2解离。
附：英文原文
Title: A mineral-based origin of Earth’s initial hydrogen peroxide and molecular oxygen
Author: He, Hongping, Wu, Xiao, Zhu, Jianxi, Lin, Mang, Lv, Ying, Xian, Haiyang, Yang, Yiping, Lin, Xiaoju, Li, Shan, Li, Yiliang, Teng, H. Henry, Thiemens, Mark H.
Issue&Volume: 2023-3-20
Abstract: Terrestrial reactive oxygen species (ROS) may have played a central role in the formation of oxic environments and evolution of early life. The abiotic origin of ROS on the Archean Earth has been heavily studied, and ROS are conventionally thought to have originated from H2O/CO2 dissociation. Here, we report experiments that lead to a mineral-based source of oxygen, rather than water alone. The mechanism involves ROS generation at abraded mineral–water interfaces in various geodynamic processes (e.g., water currents and earthquakes) which are active where free electrons are created via open-shell electrons and point defects, high pressure, water/ice interactions, and combinations of these processes. The experiments reported here show that quartz or silicate minerals may produce reactive oxygen-containing sites (≡SiO·, ≡SiOO·) that initially emerge in cleaving Si–O bonds in silicates and generate ROS during contact with water. Experimental isotope-labeling experiments show that the hydroxylation of the peroxy radical (≡SiOO·) is the predominant pathway for H2O2 generation. This heterogeneous ROS production chemistry allows the transfer of oxygen atoms between water and rocks and alters their isotopic compositions. This process may be pervasive in the natural environment, and mineral-based production of H2O2 and accompanying O2 could occur on Earth and potentially on other terrestrial planets, providing initial oxidants and free oxygen, and be a component in the evolution of life and planetary habitability.
DOI: 10.1073/pnas.2221984120
Source: https://www.pnas.org/doi/10.1073/pnas.2221984120