可解释机器学习与主动学习驱动的含石墨烯量子点透明热发射体设计及光伏封装应用

Interpretable machine learning and active learning-driven design of graphene quantum dot-containing transparent thermal emitters for photovoltaic encapsulation applications

  • 摘要: 透明热发射体需要兼顾高可见光透过率与辐射制冷能力,但复杂的功能材料耦合与多参数制备工艺,限制了传统试错法的优化效率。本研究采用可解释机器学习(PXML)与集成先验知识约束的主动学习方法(ALL-PV),设计了一种含石墨烯量子点(GQDs)的透明热发射体(TTEG)。通过PXML分析,筛选并优化了GQDs溶剂热生长体系中的关键反应条件及催化剂类型,优化后的GQDs(E-81)光致发光量子产率(PLQY)达到38.9%。在此基础上,以E-81和三环癸二甲醇二丙烯酸酯(DCPDA)为核心组分设计TTEG,并利用ALL-PV优化其制备工艺。结果表明,在约40万种制备工艺构成的设计空间中,仅通过5次迭代、共60组实验,即成功筛选出最优制备工艺。其荧光诱导透过率达到95.6%,并表现出优异的热管理性能。相较于商业玻璃封装器件,经TTEG封装的5 cm×5 cm晶硅太阳能电池实现了17.6%的功率转换效率提升(AM 1.5,100 mW·cm-2)。进一步地,对于41 cm×30 cm商业化晶硅太阳能电池组件,TTEG封装在连续日间光照条件下(8:00–18:30)使组件平均工作温度降低3.4°C,最大降温幅度达7°C,并使最大输出功率提升约10.8%。本研究为透明热发射体的工程化开发奠定了基础,同时彰显了多步骤、多属性材料人工智能引导设计的潜力。

     

    Abstract: Designing transparent thermal emitters requires a balance between high visible light transmittance and excellent radiative cooling performance. However, optimising performance across multiple objectives usually involves introducing various functional materials. This significantly increases the complexity of material preparation and performance regulation, making inefficient trial-and-error experimental methods inadequate to meet current demands. Furthermore, when it comes to multi-objective material design, the introduction of artificial intelligence (AI) technology necessitates a primary focus on clarifying whether the design logic of the algorithm aligns with the physicochemical mechanisms of the materials, as well as improving the efficiency of material design overall. In this study, a transparent thermal emitter incorporating graphene quantum dots (TTEG) is developed using interpretable machine learning (PXML) and an active learning framework with prior-knowledge constraints (ALL-PV). Six predictive models are established to estimate the fluorescence intensity of graphene quantum dots (GQDs). PXML is applied to identify the key factors governing model decisions and to clarify the associated physicochemical mechanisms. The results show that reaction temperature and catalyst molecular polarity play decisive roles in determining the fluorescence intensity of GQDs in solvothermal growth systems. Based on this understanding, we further optimized the reaction conditions and catalyst systems. The photoluminescence (PL) intensity of the resulting optimized sample, E-81, exceeded the highest value in the training dataset, and its photoluminescence quantum yield (PLQY) reached 38.9%. Next, the TTEG is fabricated from E-81 and tricyclodecanedimethanol diacrylate (DCPDA), with ALL-PV guiding the optimization of the preparation process. In ALL-PV, prior-knowledge constraints, the surrogate model, and the acquisition function work together to direct each round of experimental selection. Within a design space of more than 390,000 possible process combinations, this strategy locates the optimal preparation conditions after only five rounds of iteration and 60 experiments. The resulting fluorescent-particle-containing TTEG shows a transmittance of 95.6%. While exhibiting outstanding thermal management performance. Furthermore, we employed the finite-difference time-domain (FDTD) method to simulate the TTEG, revealing the physical mechanism by which GQDs induce the enhancement of TTEG transmittance. Finally, the energy-saving performance and stability of the TTEG are further evaluated. In Beijing, Kunming, and Haikou, the annual cooling energy consumption of the TTEG is 9.8, 8.75, and 11.45 MJ·m-2 lower than that of ordinary glass, respectively. Simultaneously, the TTEG exhibits excellent chemical stability (ΔTvis < 1%), thermal stability, and mechanical stability. When the TTEG is applied to solar cell encapsulation, the power conversion efficiency of a 5 cm × 5 cm crystalline silicon solar cell increased by 17.6% (AM 1.5, 100 mW·cm-2). For a 41 cm × 30 cm commercial crystalline silicon solar cell under all-day illumination conditions (8:00 AM to 6:30 PM), its average operating temperature decreased by 3.4 °C, with a maximum temperature drop of up to 7 °C, while the maximum output power increased by approximately 10.8%. This study lays the foundation for the engineering development of transparent thermal emitters and highlights the potential of AI-guided design for multi-step, multi-property materials.

     

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