氫氣對於實現2050年碳中和目標扮演重要的角色，通過捕獲大氣中的CO2與氫氣合成碳氫化合物燃料，達成減碳目的。綠色氫氣的生產方法可以分為電催化產氫和光催化產氫。在電催化中分成在陰極發生的氫氣析出反應，以及在陽極進行的氧氣析出反應，然而，電解反應中陽極OER的高活化能導致整體水分解反應速率緩慢。因此，我們提出NiFe1:4-BHT 作為在各種Ni 和Fe比例下具有最佳OER催化效率的電催化劑，改善電催化OER效率。另一方面，在光催化分解水中，觸媒效率低以及嚴重的電子電洞再結合限制氫氣的產量。為了增強ZnIn2S4的電荷分離效率，本研究提出具有壓電特性和雙空位的ZnIn2S4來提高光催化氫氣析出反應活性。然而，若想從實驗上理解背後的機制，將會面臨實驗條件以及成本的挑戰。因此，我們使用密度泛函理論計算來研究NiFe1:4-BHT 和雙種類缺陷 ZnIn2S4的高催化效率，透過原子尺度下計算，理解NiFe1:4-BHT 和雙種類缺陷 ZnIn2S4材料特性上差異所導致出色催化效率的原因，並提出可能的反應機制，進而給予水分解光電催化觸媒材料設計方向。
根據本研究結果顯示，Fe-BHT OER電催化觸媒經由摻雜Ni，將NiFe1:5-BHT的磁矩從Fe-BHT 的 1.94 μB 增加到 2.3 μB，並將 Fe 原子上 OH 的吸附能降低約 0.7 eV，同時將反應活化能降低約0.1 eV。同時，光催化產氫反應中我們發現較高的缺陷濃度會影響ZnIn2S4的性能，在10個S與4個In缺陷濃度下，ZnIn2S4電壓在[100]方向從2.4 V 增加到3.4 V。本研究提出新的光電催化劑設計方法，通過加入Ni至Fe-BHT不依靠外部磁場，使材料產生自發自旋極化改善OER活性，以及透過缺陷和壓電極化來減少電子和電洞的復合，改善光觸媒催化性能。透過自發自旋極化與壓電極化，為二維金屬有機骨架電催化觸媒和半導體光觸媒提出全新的設計觀點並提供重要的理論支持。

Hydrogen is crucial for achieving carbon neutrality by 2050, and to meet carbon reduction goals, we can synthesize hydrocarbons from produced hydrogen and captured CO2 in the air. Methods for producing green hydrogen can be classified into water electrolysis and photolysis, both encountering challenges like the high activation energy of the oxygen evolution reaction (OER) in electrocatalysis and the brief lifespan of photocarriers in photocatalysis. We propose NiFe1:4-BHT as an electrocatalyst with optimal OER catalytic efficiency under various Ni and Fe ratios and ZnIn2S4 with piezoelectric properties and dual vacancies to enhance photocatalytic hydrogen evolution reaction activity. Using Density Functional Theory (DFT) calculations to understand these materials, our study reveals that doping increases the magnetic moment of NiFe1:5-BHT, reduces OH adsorption energy on Fe atoms, and lowers reaction activation energy. In ZnIn2S4, higher defect concentrations improve performance, with the voltage increasing in the [100] direction at higher defect concentrations. These findings offer new design perspectives for photoelectrocatalysts, enhancing OER activity through spin polarization and improving photocatalytic performance via defects and piezoelectric polarization.

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