Zhimin Liu

Electrocatalytic CO ₂ reduction (CO ₂ RR) to value‐added multicarbon products using non‐copper‐based catalysts remains a major challenge, especially for selective ethanol production. Herein, we report that chiral Co ₃ O ₄ featuring strong electron spin polarization achieves a maximum ethanol Faradaic efficiency of 90% at ‐0.9 V versus NHE in KHCO ₃ electrolytes under a 30 bar CO ₂ pressure, substantially outperforming both racemic Co ₃ O ₄ and previously reported non‐copper‐based catalysts. The enhanced spin polarization in chiral Co ₃ O ₄ facilitates electron transfer and promotes the activation of the adsorbed CO ₂ , while also lowering the free energy change for C–C coupling to form *COCHO intermediate, thereby promoting ethanol production. Our work establishes spin polarization as a key determinant for efficient C–C coupling on non‐copper‐based catalysts and provides mechanistic principles for the rational design of CO ₂ RR electrocatalyst.

Electrocatalytic CO ₂ reduction (CO ₂ RR) to value‐added multicarbon products using non‐copper‐based catalysts remains a major challenge, especially for selective ethanol production. Herein, we report that chiral Co ₃ O ₄ featuring strong electron spin polarization achieves a maximum ethanol Faradaic efficiency of 90% at ‐0.9 V versus NHE in KHCO ₃ electrolytes under a 30 bar CO ₂ pressure, substantially outperforming both racemic Co ₃ O ₄ and previously reported non‐copper‐based catalysts. The enhanced spin polarization in chiral Co ₃ O ₄ facilitates electron transfer and promotes the activation of the adsorbed CO ₂ , while also lowering the free energy change for C–C coupling to form *COCHO intermediate, thereby promoting ethanol production. Our work establishes spin polarization as a key determinant for efficient C–C coupling on non‐copper‐based catalysts and provides mechanistic principles for the rational design of CO ₂ RR electrocatalyst.

Co-recycling of mixed plastic streams offers a viable opportunity to manage spent plastic mixtures and realize a circular economy. Herein, we present an internal dimethyl carbonate (DMC) circulation-promoted co-recycling of polycarbonate (PC) and polyester mixture into their monomers in methanol under mild conditions (e.g., 120 °C). In this protocol, PC is first methanolized to generate DMC and diol under the catalysis of ionic liquids (e.g., 1-butyl-3-methylimidazolium chloride ([BMIm][Cl])), and the resultant DMC participates in the subsequent degradation of polyester over the same catalyst, yielding dimethyl ester and carbonate. Furthermore, the generated carbonate is quickly converted into DMC under the experimental conditions, thus forming an internal DMC circulation. This strategy can be employed in handling mixtures of PC and polyester with various ratios using methanol, affording corresponding monomers in high yields. It provides an innovative perspective that accelerates the development of co-recycling technology for mixed plastic wastes.

A mild and green stepwise FA-driven ether cleavage strategy with facile product separation is developed for the full component recovery of PTHF based polyurethanes. The system works broadly for diverse PU composites and blends.

Chemical transformation of discarded polyesters into high‐value chemicals is of great significance for advancing circular economy and sustainable development. Herein, we report a facile and efficient strategy for one‐pot conversion of 1,4‐butanediol‐based polyesters (BDPs) via equivalent water hydrolysis. The reaction is achieved over 1‐butyl‐3‐methyl‐imidazolium chloride‐ZnCl ₂ ‐based ionic liquids ([BMIm][Zn _n Cl _{2 n  + 1} ]) under mild conditions (e.g., 120 °C), producing tetrahydrofuran (THF) and corresponding dicarboxylic acids. Among the designed ionic liquids, [BMIm][Zn ₄ Cl ₉ ] showed the optimal catalytic performance, affording dicarboxylic acids and THF in excellent yields. Moreover, the catalyst possesses excellent recyclability and can be reused for five consecutive runs without obvious activity attenuation. Mechanism investigation endorses that BDPs are first hydrolyzed to generate acyloxyl alcohol intermediates, which are further converted into THF and dicarboxylic acids through ring‐closing C─OH/C─O metathesis under the cooperation of cation‐anion pairs in the ionic liquid catalyst. This work establishes a simple, green, and novel protocol for the selective degradation and valorization of BDPs, holding great potential for practical industrial applications.

Precisely upcycling polyolefins into specific compounds remains a formidable challenge in sustainable chemistry. Here, we report a spatially confined relay catalysis strategy enabled by Ru single‐atom‐anchored MOR zeolite (Ru ₁ @MOR), which achieves a maximum C ₄ alkane selectivity of 63.4% and a production rate of 4516.4 mmol g _Ru ⁻¹ h ⁻¹ in the hydrocracking of low‐density polyethylene, outperforming reported catalysts to date. Combined AC HAADF‐STEM, solid‑state NMR, and density functional theory calculations demonstrated that isolated Ru ₁ sites are coordinatively situated on the inner surface of MOR, forming Ru─O─Si and Ru─O─Al linkages, which enhance the electrophilicity of framework Al sites and the Brønsted acidity strength of adjacent bridging hydroxyl groups, thereby endowing the catalyst with improved hydride abstraction capability while retaining the intrinsic carbenium‐ion‑mediated cracking pathway. Life‑cycle assessment further substantiates the minimal operating cost and environmental impacts of this system, and a techno‑economic projection for a 10 000‐tonne‐per‐year butane facility can yield annual alkane revenues exceeding US$1.5 million. This work provides a retrosynthesis‐inspired, atom‐economical paradigm for plastic waste valued, highlighting the role of precisely engineered single‑atom/zeolite interfaces in selectivity toward targeted hydrocarbon fractions.

Precisely upcycling polyolefins into specific compounds remains a formidable challenge in sustainable chemistry. Here, we report a spatially confined relay catalysis strategy enabled by Ru single‐atom‐anchored MOR zeolite (Ru ₁ @MOR), which achieves a maximum C ₄ alkane selectivity of 63.4% and a production rate of 4516.4 mmol g _Ru ⁻¹ h ⁻¹ in the hydrocracking of low‐density polyethylene, outperforming reported catalysts to date. Combined AC HAADF‐STEM, solid‑state NMR, and density functional theory calculations demonstrated that isolated Ru ₁ sites are coordinatively situated on the inner surface of MOR, forming Ru─O─Si and Ru─O─Al linkages, which enhance the electrophilicity of framework Al sites and the Brønsted acidity strength of adjacent bridging hydroxyl groups, thereby endowing the catalyst with improved hydride abstraction capability while retaining the intrinsic carbenium‐ion‑mediated cracking pathway. Life‑cycle assessment further substantiates the minimal operating cost and environmental impacts of this system, and a techno‑economic projection for a 10 000‐tonne‐per‐year butane facility can yield annual alkane revenues exceeding US$1.5 million. This work provides a retrosynthesis‐inspired, atom‐economical paradigm for plastic waste valued, highlighting the role of precisely engineered single‑atom/zeolite interfaces in selectivity toward targeted hydrocarbon fractions.

An effective strategy for selective cleavage of the C _sp2 –O and C _Ar –C _sp3 bonds in BPA-PC using a catalytic system of RuCl ₃ /triphos/In(OTf) ₃ in ethanol, and the yields of phenol and 4-isopropylphenol reached up to 99%.

The global plastic pollution issues demand transformative upcycling technologies. As a kind of advanced material, well‐defined heterocatalysts (WDHCs), which encompass well‐defined nanoparticles, sub‐nanoclusters, and atomically dispersed single‐atom catalysts, have been widely employed in the chemical transformation of various waste plastics, showing high performance due to their unique structures. This review article summarizes advances on WDHCs for plastic upcycling, focusing on the structure‐activity relationship of WDHCs and catalytic mechanisms. A framework of rational design for various WDHCs is first established, concentrating on the strategic engineering of metal centers, coordination environments, and support interfaces. Subsequently, the applications of WDHCs in catalyzing degradation of plastics via thermo‐, photo‐, and thermo‐electronic strategies are introduced in sequence, with emphasis on mechanistic insights and structure‐activity relationships of WDHCs. A critical assessment of catalyst stability, deactivation pathways, and performance in realistic mixed‐plastic feeds is integrated throughout. Finally, the challenges related to scalable synthesis of catalysts and their stability, together with process integration, are addressed, offering perspectives on the development of sustainable and industrially viable plastic upcycling technologies. This work aims to serve as a foundational reference and a design guide for the next generation of high‐performance WDHCs in enabling a circular economy of post‐consumer plastics.