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One-pot synthesis of pH-responsive charge-switchable PEGylated nanoscale coordination polymers for improved cancer therapy Yu Yang 1 , Ligeng Xu 2 , Wenjun Zhu 2 , Liangzhu Feng 1 , Jingjing Liu 2 , Qian Chen 2 , Ziliang Dong 2 , Jiayue Zhao 2 , Zhuang Liu 2 *, Meiwan Chen 1 * 1 State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Macau, China 2 Institute of Functional Nano & Soft Materials Laboratory (FUNSOM), Soochow University, Suzhou, Jiangsu 215123, China Figure S1. The UV-vis-NIR spectrum of Ca/Pt(IV)@pHis-PEG S1

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One-pot synthesis of pH-responsive charge-switchable PEGylated nanoscale coordination

polymers for improved cancer therapy

Yu Yang1, Ligeng Xu2, Wenjun Zhu2, Liangzhu Feng1, Jingjing Liu2, Qian Chen2, Ziliang Dong2, Jiayue Zhao2, Zhuang Liu2*, Meiwan Chen1*

1 State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Macau, China

2 Institute of Functional Nano & Soft Materials Laboratory (FUNSOM), Soochow University, Suzhou, Jiangsu 215123, China

Figure S1. The UV-vis-NIR spectrum of Ca/Pt(IV)@pHis-PEG

Figure S2. The EDX spectrum of Ca/Pt(IV)@pHis-PEG under the STEM pattern.

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Figure S3. The Powder X-ray diffraction (PXRD) patterns of Ca/Pt(IV) and Ca/Pt(IV)@pHis-PEG.

Figure S4. N2 adsorption/desorption isotherms of Ca/Pt(IV)@pHis-PEG.

Figure S5. The EDX of different NCPs synthesized by our method under the STEM pattern.

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Figure S6. The time-dependent (left) and concentration-dependent (right) recovery of singlet oxygen sensor green

(SOSG) fluorescence under light exposure (661 nm, 5 mW/cm2 ) of Hf-TCPP@pHis-PEG to demonstrate the

photodynamic capability of those photosensitizer-containing NCPs.

Figure S7.TEM images and DLS-measured diameters of Ca@pHis-PEG prepared by simply mixing CaCl2 with

pHis-PEG without adding other organic ligands.

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Figure S8. (a) Photographs of Ca/Pt(IV)@pHis-PEG before and after 24-hour incubation in PBS at pH 7.4 DLS-

measured hydrodynamic sizes of Ca/Pt(IV)@pHis-PEG treated PBS buffer and DMEM cell culture medium at

different time points.

Figure S9. Hydrodynamic diameter, UV-vis absorption spectrum and fluorescence spectrum of FITC-labeled Ca-

Pt(IV)@pHis-PEG.

Figure S10. Hydrodynamic diameter, UV-vis absorption spectrum and fluorescence spectrum of ICG-labeled Ca-

Pt(IV)@pHis-PEG.

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Figure S11. The stability test of FITC or ICG labled Ca-Pt(IV)@pHis-PEG incubated in cell culture medium at

various time points.

Figure S12. Photographs of mice after receiving various treatments taken at different time points during treatment.

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Figure S13. Micrographs of H&E stained major organs collected from mice treated with PBS (upper) or Ca-

Pt(IV)@pHis-PEG (below) at the end of our treatment process.

Figure S14. UV-vis-NIR absorbance of HAS-Croc incubated in buffers with different pH values.

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