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RESEARCH PAPER · Journal of the American Chemical Society · 2022

Size-Controlled Nanoparticles Embedded in a Mesoporous Architecture Leading to Efficient and Selective Hydrogenolysis of Polyolefins

Xun Wei Wu, Akalanka Tennakoon, Ryan D. Yappert, Michaela Esveld, Magali S. Ferrandon, Ryan A. Hackler, Anne M. LaPointe, Andreas Heyden, Massimiliano Delferro, Baron Peters, Aaron David Sadow, Wenyu Huang

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Size-Controlled Nanoparticles Embedded in a Mesoporous Architecture Leading to Efficient and Selective Hydrogenolysis of PolyolefinsOriginalPopulation balance models for polymer upcycling: signatures of the mechanism in the molecular weight evolution22Upcycling Plastic Wastes into Value‐Added Products by Heterogeneous Catalysis112Artificial enzymic architecture for catalytic polyolefin upcycling3Catalytic Upcycling of Plastic Waste into High Value-added Chemicals0Mason–Weaver theory: Revised and extended for a semi-infinite domain4Sustainably Recycling and Upcycling of Single-Use Plastic Wastes through Heterogeneous Catalysis32Processive Depolymerization Catalysts: A Population Balance Model for Chemistry’s “While” Loop19Dual-Pathway Polyolefin Upcycling over an Unexpectedly Bifunctional Low-Loading Ru/TiO2-Anatase Catalyst54Mechanistic classification and benchmarking of polyolefin depolymerization over silica-alumina-based catalysts143Paths to sustainable plastic waste recycling45Enabling resource circularity through thermo-catalytic and solvent-based conversion of waste plastics49RETRACTED: Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts72Competing Time Scales in Surface-Driven Solution Depolymerization2Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals94Polyethylene in Dead-End Silica Nanopores: Forces and Mobility from Non-Equilibrium Statistical Mechanics and Exchange Spectroscopy Nuclear Magnetic Resonance6Enhanced Production of Liquid Alkanes from Waste Polyethylene via the Electronic Effect‐Favored Csecondary−Csecondary Bond Cleavage42IrO2 clusters loaded on dendritic mesoporous silica nanospheres with superior peroxidase-like activity for sensitive detection of acetylcholinesterase and its inhibitors20Green synthesis of silver@graphene oxide nanocomposite for antibacterial, cytotoxicity assessment, and hydrogen peroxide electro-sensing43Site-Selective Polyolefin Hydrogenolysis on Atomic Ru for Methanation Suppression and Liquid Fuel Production90Converting Plastic Wastes to Naphtha for Closing the Plastic Loop187Coarse-Grained Modeling of Polymer Cleavage within a Porous Catalytic Support12Ultrasmall amorphous zirconia nanoparticles catalyse polyolefin hydrogenolysis176Metal-catalyzed plastic depolymerization79Recent Advances in Catalytic Chemical Recycling of Polyolefins104Mass transfer in catalytic depolymerization: External effectiveness factors and serendipitous processivity in stagnant and stirred melts31Highly Selective Catalytic Oxi‐upcycling of Polyethylene to Aliphatic Dicarboxylic Acid under a Mild Hydrogen‐Free Process7Highly Selective Catalytic Oxi‐upcycling of Polyethylene to Aliphatic Dicarboxylic Acid under a Mild Hydrogen‐Free Process73Molecular-Weight-Dependent Infiltration and Adsorption of Polymers into Nanochannels10Mechanistic Insights into Processive Polyethylene Hydrogenolysis throughIn SituNMR25Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons171Investigation into the Reaction Pathways and Catalyst Deactivation for Polyethylene Hydrogenolysis over Silica-Supported Cobalt Catalysts58Upcycling of polyvinyl chloride to hydrocarbon waxes via dechlorination and catalytic hydrogenation50A Triazole‐Based Covalent Gel Loaded with Cu/Pd Bimetallic Nanoparticles for Efficient Catalytic Cross‐Coupling Reactions4Upcycling of polyethylenes by catalysis0Ni-catalyzed carbon–carbon bonds cleavage of mixed polyolefin plastics waste42Two Mesoporous Domains Are Better Than One for Catalytic Deconstruction of Polyolefins62The cactus bulb-shaped metal-S-C/N nanoparticles supported by highly conductive channels for efficient electrocatalytic hydrogen evolution reaction4Catalisadores de rênio multivalentes aplicados a hidrogenação de CO>sub<2>/sub< em condições supercríticas0Investigating the influence of Ru structures and supports on hydrogenolysis of polyethylene plastic waste41Entropy Confinement Promotes Hydrogenolysis Activity for Polyethylene Upcycling72Entropy Confinement Promotes Hydrogenolysis Activity for Polyethylene Upcycling8Boosting the catalytic performance of metal–zeolite catalysts in the hydrocracking of polyolefin wastes by optimizing the nanoscale proximity56Effect of chloride salts and microwaves on polyethylene terephthalate (PET) hydrolysis by iron chloride/acetic acid Lewis/Brønsted acidic deep eutectic solvent15Influence of Pore Length on Hydrogenolysis of Polyethylene within a Mesoporous Support Architecture17Precise activation of C–C bonds for recycling and upcycling of plastics81Isoreticular Metal–Organic Frameworks Confined Mononuclear Ru-Hydrides Enable Highly Efficient Shape-Selective Hydrogenolysis of Polyolefins39Boosting strong metal-support interactions between Ru and sodium titanate nanowire for hydrogenolysis of polyolefins under mild conditions44A multiscale investigation of polypropylene glycol polymer upcycling to propionaldehyde via catalytic cracking on acid sites of mesoporous Y zeolites2Opportunities and challenges for plastic depolymerization by biomimetic catalysis36Synergistic catalysis for promoting selective C–C/C–O cleavage in plastic waste: structure–activity relationship and rational design of heterogeneous catalysts for liquid hydrocarbon production18Controlling Product Distribution of Polyethylene Hydrogenolysis Using Bimetallic RuM3 (M = Fe, Co, Ni) Catalysts28Polyethylene Upgrading to Liquid Fuels Boosted by Atomic Ce Promoters74Polyethylene Upgrading to Liquid Fuels Boosted by Atomic Ce Promoters21Review on Catalytic Depolymerization of Polyolefin Waste by Hydrogenolysis: State-of-the-Art and Outlook57Catalytic Hydrogenolysis of Polyethylene Under Reactive Separation46Probing Interactions between Adsorbed Polymers and γ-Al2O3 Using Solid-State NMR5Highly Selective Upgrading of Polyethylene into Light Aromatics via a Low-Temperature Melting-Catalysis Strategy55Catalytic conversion of mixed polyolefins under mild atmospheric pressure48Population Balance Equations for Reactive Separation in Polymer Upcycling20Size and Structure Effects of Carbon-Supported Ruthenium Nanoparticles on Waste Polypropylene Hydrogenolysis Activity, Selectivity, and Product Microstructure40Upcycling Waste Plastics with a C–C Backbone by Heterogeneous Catalysis45Catalytic Strategies for the Upcycling of Polyolefin Plastic Waste30Highly Selective and Efficient Perdeuteration of n‐Pentane via H/D Exchange Catalyzed by a Silica‐Supported Hafnium‐Iridium Bimetallic Complex12Highly Selective and Efficient Perdeuteration of n‐Pentane via H/D Exchange Catalyzed by a Silica‐Supported Hafnium‐Iridium Bimetallic Complex3Supported Platinum Nanoparticles Catalyzed Carbon–Carbon Bond Cleavage of Polyolefins: Role of the Oxide Support Acidity27Stable Interfacial Ruthenium Species for Highly Efficient Polyolefin Upcycling104The Overlooked Potential of Sulfated Zirconia: Reexamining Solid Superacidity Toward the Controlled Depolymerization of Polyolefins11Catalytic hydrogenolysis of polypropylene and polyethylene mixtures: Effect of temperature on liquid alkane components18Space-confined nanozyme with cascade reaction based on PCN-224 for synergistic bacterial infection treatment and NIR fluorescence imaging of wound bacterial infections35Layered Double Hydroxide Derivatives for Polyolefin Upcycling103Complete hydrogenolysis of mixed plastic wastes101Selective Upcycling of Polyethylene over Ru/H‐ZSM‐5 Bifunctional Catalyst into High‐Quality Liquid Fuel at Mild Conditions31Nanocavity in hollow sandwiched catalysts as substrate regulator for boosting hydrodeoxygenation of biomass-derived carbonyl compounds16i PP/HDPE blends compatibilized by a polyester: An unconventional concept to valuable products25Chemical Upcycling of Polyolefin Plastics Using Structurally Well-defined Catalysts35Influence of Autoclave Liner on Polyethylene Hydrogenolysis Selectivity7Catalytic chemical recycling and upcycling of polyolefin plastics27Polyethylene hydrogenolysis over bimetallic catalyst with suppression of methane formation15Encapsulated Pt-based nanoparticles for catalysis31Constructing the Al deficiency in Si-O(H)-Al units based on Pt/ZSM-5 for enhanced hydrocracking of polyethylene into high-quality liquid fuel20Synthesis and characterization of biowaste-derived porous carbon supported palladium: a systematic study as a heterogeneous catalyst for the reduction of nitroarenes5Insight into the Competitive Adsorption Behavior of Polymer Chains in Silica Nanopores by Small-Angle Neutron Scattering3Catalytic Upcycling of Polyolefins316The role of size and structure of catalytic active sites in polyolefin hydrogenolysis12Highly dispersed Ag nanocrystals functionalized ZIF-8 derived ZnO hollow structures for superior sensitive and selective detection of nitric oxide21Application of Drug Delivery System Based on Nanozyme Cascade Technology in Chronic Wound22Nonmonotonic Impact of Statistical Copolymer Composition on the Kinetics of Capillary Rise Infiltration4Efficient Hydrogenolysis of Consumer-Grade High-Density Polyethylene Wastes over MgAl-Layered Double Oxide-Supported Ru Catalysts11Unraveling the role of water in mechanism changes for economically viable catalytic plastic upcycling43Polyethylene hydrogenolysis by dilute RuPt alloy to achieve H2-pressure-independent low methane selectivity70Kinetic Models for Polymer Upcycling by Tag-and-Cut Strategies6Core–Shell Magnetic Particles: Tailored Synthesis and Applications100Reaction engineering of the hydrogenolysis of liquid n-Alkanes: Comparison of flow and batch reaction systems2Effective production of liquid/wax fuels from polyethylene plastics using Ru/Al 2 O 3 catalysts10Highly energy-efficient hydrogenolysis of high-density polyethylene via hydrogen nonthermal plasma reaction engineering4Recent developments in recycling of post-consumer polyethylene waste33Selective hydrocracking of polyolefin waste into branched liquid fuels over a non-noble metal bifunctional Ni–W/ZrO 2 catalyst4Synergistic effect of acidic sites and mesoporous confinement in Ce-doped Ru/SBA-15 catalysts for efficient hydrogenolysis of low-density polyethylene to liquid fuels7Upgrading of waste polyolefins with non-noble metal catalysts21Size‐Controlled Ni Nanoparticles Confined into Amino‐Modified Mesoporous Silica for Efficient Hydrodeoxygenation of Bio‐Derived Aromatic Aldehyde34Mechanistic Insights into Polypropylene Hydrogenolysis Using Ni/Al2O3 Catalysts17Size-Controlled Synthesis of Rhodium Nanocatalysts and Applications in Low-Temperature Hydroformylation1Tandem Catalysis for Plastic Depolymerization: In Situ Hydrogen Generation via Methanol Aqueous Phase Reforming for Sustainable Polyethylene Hydrogenolysis2Tandem Catalysis for Plastic Depolymerization: In Situ Hydrogen Generation via Methanol Aqueous Phase Reforming for Sustainable Polyethylene Hydrogenolysis27Nanoconfinement-guided in situ co-deposition of single-atom cascade nanozymes combined with injectable sodium alginate hydrogels for enhanced diabetic wound healing10Highly selective upcycling of plastic mixture waste by microwave-assisted catalysis over Zn/b-ZnO68Surface and Interface Engineering of Electrospun Nanofibers for Heterogeneous Catalysts6Advances and Challenges in Low‐Temperature Upcycling of Waste Polyolefins via Tandem Catalysis25Advances and Challenges in Low‐Temperature Upcycling of Waste Polyolefins via Tandem Catalysis2Efficient Upcycling of Polyolefin Waste to Light Aromatics via Coupling C─C Scission and Carbonylation26Efficient Upcycling of Polyolefin Waste to Light Aromatics via Coupling C─C Scission and Carbonylation5Reductive Upcycling of Polyolefins, Polyesters and Mixed Plastic Wastes to Valuable Chemicals: Bridging Chemical Catalysis With Plastic Waste Management35Upcycling polyolefins to methane-free liquid fuel by a Ru1-ZrO2 catalyst47Hydrocracking of Polyethylene to Gasoline-Range Hydrocarbons over a Ruthenium-Zeolite Bifunctional Catalyst System with Optimal Synergy of Metal and Acid Sites9Polyolefin Recycling with Binary Cobalt–Nickel Nanosheets6MOF Catalysts for Plastic Depolymerization4MOF Catalysts for Plastic Depolymerization52Synergistic Catalysis for Recycling and Upcycling of Plastics35Predicting a generalized mechanism of branched alkane hydrogenolysis on Ru, Ir, and Pt surfaces relevant to polymer upcycling applications3Population Balance Models for Catalytic Depolymerization: From Elementary Steps to Multiphase Reactors8Coordinating cracking and hydrogenation of polyethylene waste via acid-metal site isolation for selective hydrocarbon production10Catalytic Upcycling of Polyethylene into Naphtha Using Commercial Heterogeneous Catalysts3Recent Advances in the Thermo-Catalytic Upcycling of Polyethylene Waste13Polyethylene Hydrogenolysis over Ru Supported on Mesoporous MFI Zeolite: Effects of Mesoporosity and External Acid Sites16In-line NMR guided orthogonal transformation of real-life plastics63Rational design of zeolite-based composite catalysts in catalytic cracking of polyethylene6Mechanistic alteration of polyethylene oxidation via heterogenous catalysis for enhanced fatty di-carboxylic acid yields6Diffusion-mediated passing of molecular species in linear nanopores constrained by orientational alignment2Methods for Carbon Mass Closure in Polyolefin Hydrocracking6Noble Metal‐Free Low‐Temperature Aromatization of Polyethylene Waste for High‐Quality Fuel Production8Noble Metal‐Free Low‐Temperature Aromatization of Polyethylene Waste for High‐Quality Fuel Production3CO-promoted polyethylene hydrogenolysis with renewable formic acid as hydrogen donor20Dual-catalyst system without supported metals toward polyethylene waste upcycling3The silent partner in catalysis: How support architectures dictate efficiency in polyolefin hydrogenolysis1Net-Zero Upcycling of Mixed Polyolefins by Spatially Homogeneous Joule Heating7Polymer Upcycling by Catalytic Hydrogenolysis: The Role of Polyolefin Short-Chain Branching3Orchestrating catalytic hotspots and macromolecular architectures: molecular engineering toward zero-waste polymer circularity4Monitoring Depolymerization in Mesopores Using Dynamic Properties of Polymeric Melt Accessed via Dielectric Spectroscopy0Synergy Effects in a Bimetallic Ru ─ Pt Alloy Catalyst for Low‐H 2 ‐Pressure Hydrogenolysis of Low‐Density Polyethylene3Surface and Interface Properties of Metal Species for Waste Plastic Hydroconversion6Entropy Engineering for the Efficient Hydrogenolysis of Waste Polyolefins1Mechanistic insights into plastic degradation via catalytic bond breaking: a comprehensive review1Carbon–carbon bond cleavage for lignin and plastics deconstruction0Highly selective production of gasoline-range hydrocarbons via hydroconversion of polyolefins over Ru/CeO 2 and BEA hybrid catalysts0Synergistic pore-acidity engineering of hierarchical ZSM-5 for hydrogen-free upcycling of Polyethylene to C8–C12 Methylated Aromatics1Hydrocracking Polyolefins to Jet Fuel over a NiW/WO x Catalyst2A semi-flow reactor design diverts catalytic hydrogenolysis of polyolefins to metastable kinetic products1Rational design of bifunctional catalysts for hydrocracking of polyethylene waste plastics to narrow-distributed liquid fuels4Recent advancements in catalytic processes for plastic upcycling into fuels: a major step in sustainable waste management and energy production3Thermo-chemical upgrading of waste polyethylene and polypropylene plastics0

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