Exposing coordination-unsaturated Co sites in Co-MOF for efficient photocatalytic water oxidation,Inorganic Chemistry Frontiers

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Exposing coordination-unsaturated Co sites in Co-MOF for efficient photocatalytic water oxidation
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2024-07-22 , DOI: 10.1039/d4qi00968a
Jie-Yi Zhou ₁ , Xin-Yu Guan ₁ , Hui-Ping Zhang ₁ , Dong Luo ₁ , Xusheng Wang _{2,

3} , Xiao-Ping Zhou ₁ , Dan Li ₁

Affiliation

Water oxidation to molecular dioxygen driven by visible light is essential but difficult in solar fuel production due to its sluggish reaction kinetics. Although the catalytic process is highly dependent on the coordination-unsaturated metal sites in coordination catalysts, the controllable design of catalysts with such catalytic sites remains challenging. Herein, we report two new Co-MOFs (CoBIM-1 and CoBIM-2) for photocatalytic water oxidation under visible light. The coordination environment of Co in Co-MOFs can be easily manipulated by changing the atmosphere and concentration of deprotonated solvent during synthesis. CoBIM-1 with coordinatively unsaturated Co sites showed good performance with an O₂ production of 2.0 mmol g⁻¹ h⁻¹, in sharp contrast to its counterpart CoBIM-2. Furthermore, through isotope tracing experiments, we confirmed that the dioxygen was produced from water oxidation. This work highlights that the atmosphere during synthesis and solvent selection greatly regulate the crystal structures of MOFs and further manipulate their photocatalytic performance.

中文翻译：

暴露Co-MOF中的配位不饱和Co位点以实现高效光催化水氧化

可见光驱动的水氧化成分子氧在太阳能燃料生产中是必要的，但由于其反应动力学缓慢而困难。尽管催化过程高度依赖于配位催化剂中的配位不饱和金属位点，但具有此类催化位点的催化剂的可控设计仍然具有挑战性。在此，我们报告了两种用于可见光下光催化水氧化的新型Co-MOF（CoBIM-1和CoBIM-2）。通过改变合成过程中的气氛和去质子化溶剂的浓度，可以轻松控制 Co-MOF 中 Co 的配位环境。具有配位不饱和 Co 位点的 CoBIM-1 显示出良好的性能，O ₂ 产量为 2.0 mmol g ⁻¹ h ⁻¹ ，与其对应的 CoBIM- 形成鲜明对比2.此外，通过同位素示踪实验，我们证实分子氧是由水氧化产生的。这项工作强调，合成和溶剂选择过程中的气氛极大地调节了 MOF 的晶体结构，并进一步控制了它们的光催化性能。

更新日期：2024-07-25

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