隨著現代人對於健康管理的需求升高，進而推動了即時監控生理狀態的需求，透過穿戴
型生醫感測器持續監控人體生理狀態能有效幫助使用者採取預防措施並進一步防止相關併發
症。近年來以非侵入方式搜集人體體液中的特定生物標記物進行生理監測之電化學感測器的
發展在近期備受矚目，而乳酸在眾多生理資訊中為人體劇烈運動下無氧呼吸之產物，因此藉
由監測汗液中乳酸含量對於非侵入式監控人體缺氧程度是至關重要的。在眾多乳酸感測催化
材料中，酵素型感測器被廣泛應用於乳酸感測中，然而酵素型感測器在常溫情況下操作會有
容易失去活性與酵素的成本過高等問題，因此為了解決上述問題並進一步實現非侵入式診斷，
設計新型電催化觸媒應用於非酵素型電化學乳酸感測器為重要的目標之一。
有鑑於此，為了提高穿戴式非酵素型汗液乳酸感測器之靈敏度，在本論文的第四章提出
通過氮摻雜石墨烯量子點修飾金屬有機框架衍伸鎳鈷層狀雙氫氧化物(NGQD/m-NiCo-LDH)
提升其乳酸感測能力。透過 X 射線吸收光譜證明氮摻雜石墨烯量子點可以修飾金屬框架衍伸
鎳鈷層狀雙氫氧化物中過渡金屬的局域電子結構，從而降低電荷轉移阻力並加速電化學反應
過程中的電子轉移。在最適化氮摻雜石墨烯量子點之添加量後，NGQD/m-NiCo-LDH 證明其
對乳酸濃度範圍 0 至 15 mM 之感測靈敏度(62.63 ± 1.50 uA mM-1
cm-2
)高於一般鎳鈷層狀雙氫
氧化物(NiCo-LDH, 16.77 ± 1.70 uA mM-1
cm-2
)與金屬框架衍伸鎳鈷層狀雙氫氧化物(m-NiCoLDH, 45.45 ± 4.39 uA mM-1
cm-2
)並同時兼具極佳的選擇率、連續操作穩定性與重複使用性。
本研究為了更進一步調控金屬有機框架衍伸鎳鈷層狀雙氫氧化物中過度金屬價態與配位
提升此材料對於乳酸電催化反應之效能，本論文的第五章提出調控鎳鈷雙元過渡金屬比例之
金屬有機框架衍伸鎳鈷氫氧化物(m-NiCo)並應用於汗液乳酸感測。由研究結果可發現 m-NiCo
之金屬比例可以藉由金屬前驅物比例來調控，且 m-NiCo 的晶相會隨著鈷比例上升而逐漸從
具有高乳酸催化活性的-type 逐漸轉為較低催化活性的-type，進而降低了 m-NiCo 對於乳酸
感測之靈敏度。本研究針對-type 的 m-NiCo 更進一步探討雙元過度金屬比例對於金屬價態
與配位產生影響，透過 X 射線吸收光譜與拉曼圖譜分析，在最適化雙元過渡金屬比例之 m-Ni5Co1 與其他比例相比，其具有混合八面體與四面體結構以及高氧化鎳金屬價態將有助於提
升乳酸電催化反應進而提升靈敏度，在乳酸濃度範圍 0 至 12.5 mM 相較於未調控雙元金屬比
之 m-Ni1Co1 (40.11 ± 3.24 uA mM-1 cm-2)具有更出色的感測靈敏度(63.66 ± 3.86 uA mM-1
cm-2)，
且對人體汗液中常見的物質具有極佳的選擇率和優異的連續操作穩定性與重複使用性。綜合
上述所示，本研究結果說明 NGQD/m-NiCo-LDH 與最適化雙元過渡金屬比例之 m-NiCo 是具
有潛力並可應用於非酵素型電化學乳酸感測器之電催化材料。

Rapid interest in identifying specific biomarkers has been sparked by the development of
wearable electrochemical sensors for physiological and biological monitoring via non-invasive
measurement. During anaerobic metabolic circumstances, monitoring the lactate content becomes
critical for noninvasive diagnosis of hypoxia. Enzyme-based sensors are widely used in lactate
sensing among a variety of catalysts. However, enzyme-based sensors are limited due to the lack of
stability and high cost. Therefore, it is crucial to develop non-enzymatic electrochemical lactate
sensors.
To improve the sensitivity of wearable sweat biosensors for detecting lactate concentrations,
metal-organic framework (MOF) derived NiCo-based layered double hydroxides (m-NiCo LDH)
with N-doped graphene quantum dots (NGQD) decoration is designed in Chapter 4. According to
the X-ray absorption spectroscopy (XAS) analysis, the incorporation of NGQD will alter the local
electronic structure of transition metals in m-NiCo LDH, thereby reducing charge transfer resistance
and accelerating the electron transfer kinetics during electrochemical reactions of lactate detection.
After understanding the role of NGQD in the matrix of m-NiCo LDH, an as-designed NGQD/m-NiCo
LDH based electrochemical biosensor for lactate detection displayed superior sensitivity of 62.63 ±
1.50 uA mM-1
cm-2
under an applied potential of 0.60 V (vs. Ag/AgCl/3 M KCl) with the lactate
concentration range of 0 to 15 mM in alkaline condition, compared to the pristine NiCo LDH (16.77
± 1.70 uA mM-1
cm-2
) and m-NiCo LDH (45.45 ± 4.39 uA mM-1
cm-2
) based one. This research
provides a potential electrocatalyst of NGQD modified MOF derived LDH for using enzyme-free
electrochemical lactate sensors with reliable and stable performance in order to implement noninvasive human perspiration monitoring on wearable bioelectronics.
In Chapter 5, we propose to tune the valence state of Ni and coordination in m-NiCo via tuning
ratio of Ni and Co in order to improve lactate detection. The results demonstrate that metal content
can be adjusted by tuning the precursor molar ratio. In addition, the NiCo-MOF had been transformed to -type hydroxide with Co increase, which further inhibits the sensitivity toward lactate detection.
According to the XAS analysis and Raman spectrum, m-Ni5Co1 with -type hydroxide mixed
octahedral(Oh)/tetrahedral(Td) structure, exhibited an outstanding sensitivity toward lactate detection
in comparison with other m-Ni1Co1. As intended, the m-Ni5Co1-based electrochemical biosensor
for lactate detection exhibited a superior sensitivity of 63.66 ± 3.86 uA mM-1
in comparison with mNi1Co1(40.11 ± 3.24 uA mM-1
cm-2
) with a lactate concentration range of 0 to 12.5 mM under
alkaline medium. This study proposes an innovative category of electrocatalysts for use in nonenzymatic electrochemical lactate sensors with dependable and stable performance as one of the noninvasive biosensors

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