雙金屬二維π–d共軛苯六硫醇 (Benzenehexathiol, BHT) 框架近年來被視為具潛力的氧氣析出反應 (Oxygen evolution reaction, OER) 電催化平台。然而，其多組合的組成空間使實驗篩選相當耗時，而基於計算氫電極 (Computational hydrogen electrode, CHE) 的自由能排序亦容易受到溶劑效應與外加電位影響，限制其預測可靠性。因此，本研究避免僅依賴單一反應自由能變化作為篩選依據，改以局部磁矩、*OH吸附行為、穩定性與導電性等多項特徵進行綜合評估。基於我們先前對NiFe-BHT的實驗與理論研究，本研究利用密度泛函理論Density functional theory, DFT) 系統性探討單金屬TM–BHT及錳基雙金屬MnTM–BHT (TM = Fe、Co、Ni、Cu) 的催化特性。結果顯示，MnFe5:1-BHT能在保留較高Mn局部磁矩 (2.757 μB) 的同時，將Mn位點的*OH吸附能 (Ead) 調控至較有利的負值區域 (−0.647 eV) 。計算氫電極 (CHE) 分析定性指出Fe與Mn之間存在協同作用，其中Fe對鄰近Mn位點具有電子調控效果。此外，透過熱力學穩定性與玻爾茲曼輸運計算分析，MnFe5:1-BHT具有與已合成單金屬BHT相近的亞穩定性及足夠的導電能力。綜合多項電子結構與材料性質分析，本研究提出MnFe5:1-BHT為具實驗潛力之OER催化候選材料。

Bimetallic two-dimensional π–d conjugated benzenehexathiol (BHT) frameworks have attracted increasing attention as potential electrocatalysts for the oxygen evolution reaction (OER). Nevertheless, the large number of possible metal combinations makes experimental exploration inefficient, and activity predictions based solely on computational hydrogen electrode (CHE) free-energy profiles may be influenced by solvation effects and applied potentials. To address these limitations, this study adopts a multi-property evaluation strategy rather than relying on a single reaction free-energy change. Density functional theory (DFT) calculations were performed to examine monometallic TM–BHT frameworks and Mn-based bimetallic MnTM–BHT systems, where TM = Fe, Co, Ni, and Cu. The results show that Fe incorporation into Mn-BHT effectively modifies the adsorption behavior of the Mn site. In particular, MnFe5:1-BHT exhibits a favorable *OH adsorption energy (Ead) of −0.647 eV while maintaining a high local Mn magnetic moment of 2.757 μB. Qualitative CHE analysis further suggests that Fe and Mn may play cooperative roles, with Fe contributing to the reaction energetics and electronically influencing neighboring Mn sites. In addition, convex-hull analysis and Boltzmann transport calculations indicate that MnFe5:1-BHT possesses metastability comparable to experimentally reported monometallic BHT frameworks and sufficient charge transport capability. Overall, the combined analysis of adsorption behavior, magnetic properties, thermodynamic stability, and electronic transport supports MnFe5:1-BHT as a promising candidate for future OER electrocatalyst development.

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