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Figure 1. Schematic diagrams of conventional PET recycling methods, petroleum-based p-TA preparation, and the new method for p-TA production via selective hydrogenation of PET in this work.

Figure 2. Optimization of reaction conditions for targeted hydrogenation of waste PET to p-TA and PX over Pt-based catalysts. (A) Effect of different supports; (B) effect of second metal sites of bimetallic Pt-M/MCM-48 (n(Pt): n(M) = 1:1.5); (C) effect of Pt/W molar ratio in PtW/MCM-48 catalyst; (D) effect of reaction temperature; (E) effect of H₂ pressure. General reaction conditions: 0.05 g PET, 3 mL of H₂O, 12 h, 700 rpm, 0.05 g catalyst with 5.0 wt% Pt loading, pH=2, 260 ï¿½ï¿½C, 2 MPa H₂.

Figure 3. (A, B) Reaction product distributions on the targeted hydrogenation of waste PET over (A) PtW_1.5/MCM-48 and (B) Pt/MCM-48 catalysts as a function of time. Reaction conditions: 0.05 g PET, 3 mL of H₂O, 260 ï¿½ï¿½C, 2 MPa H₂, 12 h, 700 rpm, 0.05 g catalyst, pH=2 (with PWA). Specially, for aromatic liquid products, the yields were calculated by (moles of aromatic ring in product)/ (moles of aromatic ring in feedstock). For raw PET materials, the conversion was calculated by (moles of all aromatic liquid products)/ (moles of aromatic ring in feedstock). (C) Possible reaction pathway for the targeted hydrogenation of waste PET over PtW_1.5/MCM-48 catalyst.

Figure 4. (A) XRD patterns of MCM-48, Pt/MCM-48 catalyst, and PtW/MCM-48 catalysts with different Pt/W molar ratios. (B) UV-vis spectra of (a) MCM-48, (b) W_1.5/MCM-48, (c) W₂/MCM-48, (d) Pt/MCM-48, (e) PtW_0.5/MCM-48, (f) PtW_1.3/MCM-48, (g) PtW_1.5/MCM-48, (h) PtW_1.8/MCM-48, (i) PtW₂/MCM-48. (C) Raman spectra of (a) MCM-48, (b) Pt/MCM-48, (c) PtW_0.5/MCM-48, (d) PtW_1.3/MCM-48, (e) PtW_1.5/MCM-48, (f) PtW_1.8/MCM-48, (g) PtW₂/MCM-48, (h) W_1.5/MCM-48, (i) W₂/MCM-48. (D) H₂-TPR profiles of the Pt/MCM-48 and PtW_1.5/MCM-48 catalysts. (E) XPS spectra of W4f in the W_1.5/MCM-48, PtW₂/MCM-48 and PtW_1.5/MCM-48 catalysts. (F, G) HAADF-STEM images of (F) W_1.5/MCM-48 and (G) W₂/MCM-48 samples. (H-K) EDX spectroscopy mapping profiles of PtW_1.5/MCM-48 catalyst. (L-N) HR-TEM images and particle size distributions of (L) PtW_1.5/MCM-48, (M) Pt/MCM-48, (N) PtW₂/MCM-48 catalysts. (O-T) HR-TEM images of the PtW_1.5/MCM-48 catalyst.

Figure 5. (A) XPS spectras of W4f in the PtW/MCM-48 catalysts with different PtW molar ratios. (B) Correlation between the molar ratio of Pt/W of PtW/MCM-48 catalysts and the formation rate of p-TA and PX, along with the W⁵⁺/(W⁵⁺+W⁶⁺) ratio on the catalysts surface. (C) NH₃-TPD profiles of the PtW/MCM-48 catalysts. (D) Relationship between Pt/W molar ratio in PtW/MCM-48 catalysts and the content of weak and total acidic sites. (E) Acetic acid TPD-MS results for PtW/MCM-48 catalysts with different PtW molar ratios. (F, G) The IR spectra of adsorbed pyridine on (F) PtW₁_.5/MCM-48 and (G) PtW₂/MCM-48 catalysts. (H) Br?nsted and Lewis acid sites contents and ratios of Pt/MCM-48 and PtW/MCM-48 catalysts.

Figure 6. (A, B) DRIFTS images of acetic acid adsorption on (A) PtW₁_.5/MCM-48 and (B) PtW₂/MCM-48 catalysts. (C, D) The intermediate CH₃-Ph-COOH* on the (C) W₃O₇/Pt(111) and (D) W₄O₇/Pt(111) model. (E) Reaction energies of the hydrogenolysis of p-TA on W₃O₇/Pt(111) and W₄O₇/Pt(111) surfaces. (F, G) Schematic diagram of selective hydrogenation of waste PET to p-TA and PX over (C) PtW₁_.5/MCM-48 and (D) PtW₂/MCM-48 catalysts.

Figure 7. (A) Targeted hydrogenation of real waste PET plastics (a) polyester rope, (b) seal bag, (c) water bottle, (d) snake-skin rope, (e) tray, (f) coloured ribbon, (g)white terylene cotton, (h)black terylene cotton to p-TA and PX over PtW₁_.5/MCM-48 catalyst. General reaction conditions: 0.05 g real PET plastics, 3 mL of H₂O, 260 ï¿½ï¿½C, 2 MPa H₂, 700 rpm, 12 h, 0.05 g PtW_1.5/MCM-48, pH=2 (with PWA). (B) Comparison of the revenues and costs of waste PET and naphtha to p-TA (100,000 tons p-TA production per year). (C) Comparison of the viabilities of the production of p-TA from waste PET and naphtha. ï¿½ï¿½M-facterï¿½ï¿½ referred as Material consumption (ton/ton p-TA) and ï¿½ï¿½C-facterï¿½ï¿½ referred as Catalyst cost ($/ton p-TA). (D) Comparison of non-renewable energy use (NREU) and global warming potential (GWP) in production of 1 kg p-TA from waste PET and naphtha.

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