Figure S1. SEM images of defect-free UIO-66 under different magnifications.

Figure S2. TEM image and EDS patterns of Zr-H-6 ml.

Figure S3. FTIR spectra of Zr-MOFs with different synthesized conditions: a) different synthesized time, b) different reaction temperature, c) preparation under different hydrochloric acid content.

Figure S4. Pore size distribution curve of Zr-MOFs and defect-free UIO-66.

Table S1. Measurement of organic elements and Zr element of Zr-H-6 ml samples calcinating at different temperatures. “1” represents treating at 80°C, “2” represents treating at 200°C, and “3” represents treating at 400°C.

Figure S5. DBT oxidation products in acetonitrile phase are detected. The catalysts were UIO-66 in different synthesized conditions: a) Zr-H-2 h, b) Zr-H-10 h, c) Zr-H-120°C, d) Zr-H-140°C, e) Zr-H-4 ml, f) Zr-H-6ml, g) Zr-H (-10 ml). Reaction conditions: temperature = 60°C; catalyst dosage = 30 mg; O/S molar ratio = 7.5:1; initial sulfur concentration = 730 ppm; reaction time = 10 min. Corresponding peak representative substance, 8.75: DBT; 11.0: DBTO2.