1：Experimental Design and Method Selection:

The study involves synthesizing multilayered Ti3C2Tx MXene by etching Ti3AlC2 with HCl and LiF, delaminating it via sonication, synthesizing cationic Azo-surfactants (AzoTMA), and fabricating the Azo-MXene hybrid through electrostatic self-assembly. Characterizations include NMR, zeta potential, SEM, TEM, XRD, UV-Vis, XPS, contact angle measurements, and electrochemical tests (CV and GCD) to analyze morphology, structure, photoresponse, and electrochemical behavior.

2：Sample Selection and Data Sources:

Samples include Ti3AlC2 for MXene synthesis, AzoC8OBr for AzoTMA synthesis, and deionized water for suspensions. Data are obtained from laboratory experiments and instrument measurements.

3：List of Experimental Equipment and Materials:

Equipment includes Varian Inova-400 NMR spectrometer, Malvern Zetasizer Nano ZS90 for zeta potential, Hitachi JSM-6700F SEM, JEOL JEM-2100F TEM, Bruker D8 XRD, Hitachi U3900 UV-Vis, PHI 5000c ESCA XPS, JC2001 contact angle goniometer, CHF-XQ-500W UV lamp, and CHI440A electrochemical workstation. Materials include Ti3AlC2, HCl, LiF, AzoC8OBr, trimethylamine, ethyl acetate, ethanol, Nafion solution, H2SO4, and deionized water.

4：Experimental Procedures and Operational Workflow:

MXene is synthesized by etching Ti3AlC2 with HCl/LiF at 35°C for 24h, followed by centrifugation and freeze-drying. Delaminated MXene is obtained by sonication in water and centrifugation. AzoTMA is synthesized by reacting AzoC8OBr with trimethylamine in ethyl acetate/ethanol at 70°C for 48h, followed by recrystallization. Azo-MXene hybrid is made by adding AzoTMA to MXene suspension, stirring overnight, washing, and filtering. Characterizations are performed as per standard protocols. Electrochemical tests use a three-electrode system with GCE, Pt wire, and SCE in 1M H2SO4 electrolyte.

5：Data Analysis Methods:

Data are analyzed using instrument software; gravimetric capacitance is calculated from GCD curves using equation C = (I * Δt) / (m * ΔV). Statistical methods include averaging contact angle measurements.