Multistep Surface Trap State Finishing Based on in Situ One-Step MOF Modification over Hematite for Dramatically Enhanced Solar Water Oxidation.,ACS Applied Materials & Interfaces

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Multistep Surface Trap State Finishing Based on in Situ One-Step MOF Modification over Hematite for Dramatically Enhanced Solar Water Oxidation.
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-07-15 , DOI: 10.1021/acsami.0c06445
Shuai Chen ₁ , Jinhua Li ₁ , Jiachen Wang ₁ , Hong Zhu ₂ , Jing Bai _{1,

3} , Yan Zhang ₁ , Tingsheng Zhou ₁ , Mengyang Zhou ₁ , Baoxue Zhou _{1,

3,

4}

Affiliation

Complex surface dynamics is the key to limit the photoelectrochemical performance of hematite, while its core content is the hole trapping and release by surface traps. Deep traps are accompanied by extremely fast capture rates and extremely slow release rates, which severely suppress the hole transport process. Herein, we proposed a unique method to progressively convert deep traps on the hematite surface for fast hole transfer via in situ one-step metal organic framework modification. This stepwise deep-trap passivation is achieved by hematite corrosion first on the surface and subsequent construction of a porous titanium layer. The gentle trap finishing helps prevent surface losses caused by excessively intense trap passivation. The hematite corrosion can initially passivate 80% of the surface deep traps, while the subsequent porous titanium layer can completely passivate the deep traps. In addition, the accurate optimization of the porous titanium layer can reconstruct the benign shallow traps on the surface, acting as superior oxygen evolution reaction active sites. This sophisticated surface-trap adjustment is accompanied by the rapid reduction of deep traps and the gradual increase of shallow traps, obtaining a superior surface state that is conducive to charge transport and interface catalysis. The obtained treated hematite yields a photocurrent density of 3.08 mA·cm^–2 at 1.23 V_RHE, increased by 570% compared to the pristine hematite.

中文翻译：

基于在赤铁矿上进行原位一步MOF改性的多步表面阱状态精加工，可显着增强太阳能氧化能力。

复杂的表面动力学是限制赤铁矿光电化学性能的关键，而其核心成分是空穴捕获和表面陷阱释放。深陷阱伴随着极快的捕获速度和极慢的释放速度，从而严重抑制了空穴传输过程。在本文中，我们提出了一种独特的方法，可通过原位一步有机金属修饰逐步转换赤铁矿表面上的深陷阱，以实现快速的空穴传输。这种逐步深陷的钝化是通过首先在表面上进行赤铁矿腐蚀并随后构造多孔钛层来实现的。捕集阱的温和处理有助于防止捕集阱钝化过度引起的表面损失。赤铁矿腐蚀最初会钝化80％的表面深层陷阱，而随后的多孔钛层可以完全钝化深陷阱。另外，对多孔钛层的精确优化可以在表面上重建良性的浅陷阱，作为优良的析氧反应活性位点。这种复杂的表面陷阱调整伴随着深陷阱的快速减少和浅陷阱的逐渐增加，从而获得了有利于电荷传输和界面催化的优越表面状态。所获得的处理过的赤铁矿的光电流密度为3.08 mA·cm 这种复杂的表面陷阱调整伴随着深陷阱的快速减少和浅陷阱的逐渐增加，从而获得了有利于电荷传输和界面催化的优越表面状态。获得的处理过的赤铁矿的光电流密度为3.08 mA·cm 这种复杂的表面陷阱调整伴随着深陷阱的快速减少和浅陷阱的逐渐增加，从而获得了有利于电荷传输和界面催化的优越表面状态。所获得的处理过的赤铁矿的光电流密度为3.08 mA·cm与原始赤铁矿相比，在1.23 V _RHE时的^–2增大了570％。

更新日期：2020-07-29

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