铁（氢氧化）氧化物的光还原溶解及其地球化学意义,ACS Earth and Space Chemistry

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铁（氢氧化）氧化物的光还原溶解及其地球化学意义
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2022-03-10 , DOI: 10.1021/acsearthspacechem.1c00334
Ying Lv _{1,

2} , Jing Liu _{1,

2,

3} , Runliang Zhu _{1,

2} , Jianxi Zhu _{1,

2} , Qingze Chen _{1,

2} , Xiaoliang Liang _{1,

2} , Hongping He _{1,

2}

Affiliation

铁（氢）氧化物是最丰富的金属氧化物，以微/纳米粒子的主要形式广泛分布在地球表面。铁（氢）氧化物的溶解显着控制了它们在地球表面的成分，是全球铁循环的关键步骤。铁（氢）氧化物的光还原溶解被认为是生成 Fe ^{2+的最重要过程之一}在地表水中，也是将太阳能转化为化学能的常见途径。这篇综述文章剖析了铁（氢）氧化物光还原溶解的主要特征，并讨论了其地球化学和环境意义。我们将铁（氢）氧化物的光还原机制分为三种类型：通过本征光生电子还原、通过配体还原为金属电子转移 (LMCT) 和通过直接注入外源光电子进行还原。光还原溶解的效率受铁（氢）氧化物的结构（例如，晶体结构和粒度）和环境条件（例如，光、pH 和同时发生的化学物质）的限制。所以，由于其独特的晶体结构和物理化学性质，不同的铁（氢）氧化物可能表现出非常独特的光还原溶解特性。结晶度低的铁（氢）氧化物（例如，水铁矿、纤铁矿）容易发生直接的光还原溶解，而结晶度高的（例如，针铁矿、赤铁矿）通常需要配体才能进行光还原溶解。铁（氢）氧化物的光还原溶解涉及许多重要的地球化学和环境过程，例如初级生产者的铁可用性、活性氧的产生、污染物的运输和归宿，以及铁（氢）的相变。 )氧化物。鉴于铁（氢）氧化物的光还原溶解无处不在，

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Photoreductive Dissolution of Iron (Hydr)oxides and Its Geochemical Significance

Iron (hydr)oxides are the most abundant metal oxides, which are widespread on Earth’s surface in the major form of micro/nanoparticles. Dissolution of iron (hydr)oxides significantly controls their compositions on Earth’s surface and is a critical step for the global Fe cycling. Photoreductive dissolution of iron (hydr)oxides is recognized as one of the most important process for generating Fe²⁺ in surface water and is also a common pathway for transforming solar energy into chemical energy. This review article dissects the main characteristics of photoreductive dissolution of iron (hydr)oxides and discusses its geochemical and environmental significance. We categorize the mechanisms for photoreduction of iron (hydr)oxides into three types: reduction by intrinsic photogenerated electrons, reduction by ligand to metal electron transfer (LMCT), and reduction by direct injection of exogenous photoelectrons. The efficiency of photoreductive dissolution is constrained by both the structure of iron (hydr)oxides (e.g., crystal structure and particle size) and environmental conditions (e.g., light, pH, and concurrent chemicals). Therefore, different iron (hydr)oxides may exhibit quite distinctive photoreductive dissolution characteristics because of their unique crystal structures and physicochemical properties. Iron (hydr)oxides with low crystallinity (e.g., ferrihydrite, lepidocrocite) are subject to direct photoreductive dissolution, while those with high crystallinity (e.g., goethite, hematite) generally need ligands to proceed with photoreductive dissolution. The photoreductive dissolution of iron (hydr)oxides is involved in many important geochemical and environmental processes, such as the Fe availability to primary producers, the generation of reactive oxygen species, the transportation and fate of contaminants, and the phase transformation of iron (hydr)oxides. Given the ubiquitous occurrence of photoreductive dissolution of iron (hydr)oxides, this review will advance our understanding of the role of this process in Earth’s surface environments.

更新日期：2022-03-10

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