能源需求的增加已經導致須通過有效地利用電解水分解的氫燃料的快速發展。然而，考慮到氧析出反應（OER）的緩慢動力學是其電化學活性的瓶頸，希望開發在鹼性條件下運行的氧析出反應之電催化觸媒。雖然貴金屬在電催化劑表現有優異的OER活性，但是其生產的高成本阻礙了其實際應用。為了解決這些局限性，開發出了具有成本效益以及地球富含量高的電催化觸媒。過渡金屬是被考慮的選項之一，由於擁有很好的電催化表現。
在各種材料中，層狀雙氫氧化物（LDH）由於其強大的電催化活性而表現出了對OER的優越性能，因此有限的活性位點阻礙了更進一步的應用。最近，透過使用具有高表面積和孔隙的前驅物模板（例如金屬有機框架材料（MOF））來製造複雜結構的形態，為了獲得所希望的特性，也提供了更多應用的可能性。最近合成具有多孔壁和大量空洞的複雜結構ZIF衍生的LDH可以通過提供更多的活性位點和模板衍生的可調性之特點來提高反應動力學。
由於這些優越的性能，ZIF-67衍生的LDH有效地促進了OER表現，但MOF-74的實際應用仍然受到限制。迄今為止，在本文中我們的目的是在鹼性溶液中自發性轉化來設計出一種新的由雙金屬MOF衍生的NiFe-LDH，並利用此方法來進一步提高其性能，因為NiFe-LDH仍然有導電性不佳的問題。
本論文分為兩部分，設計從雙金屬MOF-74自發衍生的NiFe-LDH用於鹼性溶液中氧析出反應的電催化觸媒（第4章），並通過摻入雜原子摻雜來促進MOF衍生的LDH的氧析出反應。並將其材料與碳材做結合，且進一步導入石墨烯量子點（GQD）來提升電催化的析氧反應（第5章）。
在本文的第4章中，首次提出了一種涉及雙金屬金屬有機骨架（MOF）的NiFe-LDH的簡單轉化方法，且無需施加任何額外的方法即可在鹼性電解液中通過自發衍生製備NiFe層狀雙氫氧化物（LDH）。由於雙金屬MOF-74的NiFe LDH為在鹼性溶液中電催化OER提供了理想的活性的位點，並促進了電解液在有組織的奈米結構中均勻通道內的滲透，從而進一步增加了活性物質與電解質之間的接觸面積。對於OER，在10 mA / cm2的電流密度下，從MOF-74衍生的NiFe-LDH電催化觸媒得到299 mV的過電位，低於商業化RuO2。 MOF衍生的NiFe-LDH在電流密度為10 mA / cm2時也具有24小時以上的長期穩定性。
在第5章中，我們通過摻雜的GQD摻入MOF衍生的NiFe-LDH中來開發新型催化材料，該物質可促進活性位點的暴露和足夠的活性位點來進行OER反應。 GQD具有許多邊緣和缺陷部位，在這些部位有利於進行催化反應。一些理論上創新的策略（例如雜原子摻雜）會破壞GQD的電中性，從而產生重新分佈的電荷區，為催化反應提供活性位點。摻雜GQD / MOF-74衍生的NiFe-LDH在100 mA / cm2的電流密度下得到251 mV的超低過電壓，較低的Tafel斜率34.9 mV dec-1，並且在高電流密度100 mA cm-2下，內具有24小時以上出色的穩定性。

The increase of high energy resource demand has led to the rapid development of clean fuel of hydrogen by efficiently electrolytic water splitting. However, considering the sluggish kinetics of the oxygen evolution reaction (OER) as the bottleneck in its electrochemical activity, it is desirable to develop water oxidation electrocatalysts operating under alkaline conditions. While the noble metal- based electrocatalysts exhibited superior OER activity, the scarcity and high cost hinder its practical application. To address these limitations, the development of cost-effective, earth-abundant electrocatalysts such as transition metal-based electrocatalysts have gained consideration due to their promising electrocatalytic performance. Among various materials, layered double hydroxide (LDH), had demonstrated superior performance towards OER because of their robust electroactivity, hence the limited active sites hinders its further applications. Recently, the fabrication of complex-structured morphologies by using precursor templates with high surface area and porosity, such as metal-organic framework (MOFs), let it obtained the desired properties which open more opportunities for further applications. Recent fabrication of complex-structure ZIF-derived LDH with porous walls and massive cavities favoring reaction kinetics by exposing more active sites and flexible composition feature derived from the templates. Considering these superior properties, ZIF-67 derived LDH had effectively promoted the OER activity, yet the practical application of MOF-74 are still limited. Heretofore, in this thesis, we aimed to design an evolved novel bimetallic MOF-derived-NiFe-LDH by spontaneous transformation in alkaline solution and a strategy design to further boost up its performance, as the NiFe-LDH still suffers from the lack of electronic conductivity. There are two parts of this thesis, designing a spontaneously deriving NiFe-LDH from bimetallic MOF-74 as an electrocatalyst for oxygen evolution reaction in alkaline solution (Chapter 4) and boosting oxygen evolution of MOF- derived-LDH by incorporation of heteroatom-doped graphene quantum dots (GQD). and integrating it with carbon-based materials, in which herein we used graphene quantum dots (GQD) for electrocatalytic oxygen evolution reaction (Chapter 5).
4
In the Chapter 4, herein, a facile transformation of NiFe-LDH involving bimetallic metal-organic framework (MOF) is proposed for the first time for fabricating the NiFe layered double hydroxide (LDH) via spontaneously deriving process in the alkaline electrolyte without any additional treatments. The bimetallic MOF-74-derived NiFe LDH provided desirable hot spots for electrocatalizing OER in alkaline solution and facilitated electrolyte penetration within the uniform channel in an organized nanostructure to further increase the contact area between the active material and electrolyte. The as- obtained electrocatalyst of MOF-74-derived NiFe-LDH exhibited a low overpotential of 299 mV at 10 mA/cm2 current density for OER, lower than commercial RuO2. MOF-derived-NiFe-LDH also possessed long-term stability over 24 hours at a current density of 10 mA/cm2.
In the Chapter 5, we developed novel catalytic materials by incorporation of heteroatom-doped
GQD into MOF-derived-NiFe-LDH that promotes active sites exposure, suitable spots and sufficient
active sites for hosting OER reactions. GQD has featured with numerous edge and defect sites in which
beneficial for hosting the catalytic reactions. Some theoretical innovative strategies, such as heteroatom
doping would shatter the GQD’s electroneutrality, thus creating re-distributed charge areas that provide
active sites for catalytic reactions. The as-designed heteroatom-doped GQD/MOF-74-derived NiFe-
LDH exhibited a ultralow overpotential of 251 mV at current density of 100 mA/cm2, lower Tafel slope
of 34.9 mV dec-1, and possessed excellent durability over 24 hours in high current density, 100 mA cm- 2.

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