ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3038 - 3045
Опубликована: Фев. 5, 2025
Язык: Английский
ACS Catalysis, Год журнала: 2024, Номер 14(7), С. 5366 - 5376
Опубликована: Март 26, 2024
Upcycling poly(ethylene terephthalate) (PET) waste into valuable C2 products presents an alternative avenue for attaining carbon neutrality. In this study, we introduce a C–C preserved pathway selectively transforming PET-derived ethylene glycol (EG) glycolic acid (GA), 25-fold value of product. Utilizing Pt–Ni(OH)2/NF electrode, EG oxidation reaction (EGOR) proceeds at remarkably low potential (100 mA cm–2 @0.69 V vs reversible hydrogen electrode (RHE)) with impressive Faraday efficiency (93%) GA production. situ Fourier transform infrared (FTIR) measurements are employed to pinpoint crucial intermediates, elucidating pathways the conversion GA. Quasi in electron paramagnetic resonance (EPR) experiments identify rich •OH species Pt–Ni(OH)2, making active Pt sites less susceptible be poisoned through oxidative removal adsorbed carbonyl intermediates during EGOR. Density functional theory (DFT) calculations underscore synergistic interplay between and Ni(OH)2, optimizing adsorption/desorption on metal ensuring heightened activity, selectivity, stability Furthermore, propose innovative electro-forming architecture by integrating EGOR evolution (HER) oxygen reduction (ORR). This hybrid is activated multifunctional catalytic deployed throughout day switch mode. It can achieve high-value chemical production from PET hydrolysate concurrent generation electric energy output, offering appealing multifaceted solution plastic upcycling.
Язык: Английский
Процитировано
45
Nature Communications, Год журнала: 2024, Номер 15(1)
Опубликована: Июль 19, 2024
Freshwater scarcity and microplastics (MPs) pollution are two concerning intertwined global challenges. In this work, we propose a "one stone kills birds" strategy by employing an interfacial solar evaporation platform (ISEP) combined with MPs adsorbent. This aims to produce clean water simultaneously enhance removal. Unlike traditional predecessors, our ISEP generates condensed free from contamination. Additionally, the photothermally driven separation process significantly improves removal performance. We observed ratio increase of up 5.5 times compared previously reported adsorbents. Thus, rationally-designed holds promising potential not only mitigate existing issue but also remediate in natural environments.
Язык: Английский
Процитировано
40
Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(17)
Опубликована: Апрель 17, 2024
Recently, there has been a notable surge in interest regarding reclaiming valuable chemicals from waste plastics. However, the energy-intensive conventional thermal catalysis does not align with concept of sustainable development. Herein, we report electrocatalytic approach allowing selective synthesis glycolic acid (GA) polyethylene terephthalate (PET) over Pd 67 Ag 33 alloy catalyst under ambient conditions. Notably, delivers high mass activity 9.7 A mg −1 for ethylene glycol oxidation reaction (EGOR) and GA Faradaic efficiency 92.7 %, representing most active synthesis. In situ experiments computational simulations uncover that ligand effect induced by incorporation enhances selectivity facilitating carbonyl intermediates desorption, while lattice mismatch-triggered tensile strain optimizes adsorption *OH species to boost kinetics. This work unveils synergistic provides guidance design future catalysts PET upcycling. We further investigate versatility on CO 2 reduction (CO RR) assemble EGOR//CO RR integrated electrolyzer, presenting pioneering demonstration reforming carbon resource (i.e., ) into high-value chemicals.
Язык: Английский
Процитировано
38
Advanced Materials, Год журнала: 2024, Номер unknown
Опубликована: Июль 28, 2024
Abstract Electro‐reforming of poly(ethylene terephthalate) (PET) into valuable chemicals is garnering significant attention as it opens a mild avenue for waste resource utilization. However, achieving high activity and selectivity C2 products during ethylene glycol (EG) oxidation in PET hydrolysate on Pd electrocatalysts remains challenging. The strong interaction between carbonyl (*CO) intermediates leads to undesirable over‐oxidation poisoning sites, which hinders the highly efficient production. Herein, nonmetallic alloying strategy employed fabricate Pd‐boron alloy aerogel (PdB), wherein B atoms are induced regulate electron structure surface oxophilicity. This approach allows remarkable mass 6.71 A mg −1 , glycolic acid (GA) Faradaic efficiency (FE) 93.8%, stable 100 h cyclic electrolysis. In situ experiments density functional theory calculations reveal contributions inserted lattice effective EG‐to‐GA conversion. Interestingly, heightened oxophilicity regulated electronic by incorporation weakened *CO adsorption enhanced hydroxyl species affinity accelerate oxidative *OH adspecies formation, thereby synergistically avoiding boosting GA synthesis. work provides insights rational design high‐performance synthesis via an oxophilic motifs strategy.
Язык: Английский
Процитировано
31
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(11)
Опубликована: Янв. 10, 2024
Abstract Upgrading of polyethylene terephthalate (PET) waste into valuable oxygenated molecules is a fascinating process, yet it remains challenging. Herein, we developed two‐step strategy involving methanolysis PET to dimethyl (DMT), followed by hydrogenation DMT produce the high‐valued chemical methyl p‐methyl benzoate (MMB) using fixed‐bed reactor and Cu/ZrO 2 catalyst. Interestingly, discovered phase structure ZrO significantly regulates selectivity products. Cu supported on monoclinic (5 %Cu/m‐ZrO ) exhibits an exceptional 86 % for conversion MMB, while tetragonal %Cu/t‐ZrO predominantly produces p‐xylene (PX) with 75 %. The superior MMB over Cu/m‐ZrO can be attributed weaker acid sites present m‐ZrO compared t‐ZrO . This weak acidity leads moderate adsorption capability facilitating its desorption. Furthermore, DFT calculations reveal catalyst shows higher effective energy barrier cleavage second C−O bond Cu/t‐ZrO catalyst; this distinction ensures high MMB. not only presents approach upgrading fine chemicals but also offers controlling primary product in multistep reaction.
Язык: Английский
Процитировано
22
Coordination Chemistry Reviews, Год журнала: 2025, Номер 532, С. 216545 - 216545
Опубликована: Фев. 19, 2025
Язык: Английский
Процитировано
12
AIChE Journal, Год журнала: 2025, Номер unknown
Опубликована: Янв. 23, 2025
Abstract Photoreforming waste plastics into valuable products is a promising approach, but it requires efficient, eco‐friendly photocatalysts and deeper understanding of catalytic mechanism. We have developed B‐doped g‐C 3 N 4 nanotube catalyst with well‐defined structure for photoreforming poly(ethylene terephthalate) (PET) chemicals H 2 . This achieved evolution rate 3240 μmol g catal −1 h , outperforming previous cadmium‐free catalysts. It also oxidized PET to higher‐value organic acids via hole oxidation Experimental theoretical calculations showed that B atom doping not only greatly increased the catalyst's active sites, significantly accelerated electron–hole separation transfer rate, optimized adsorption activation behavior substrate. Using concentrated sunlight, we 475 real‐world in seawater. Techno‐economic analysis suggests processing 50,000 tons plastic annually could yield profit $7.45 million.
Язык: Английский
Процитировано
11
Advanced Materials, Год журнала: 2025, Номер unknown
Опубликована: Янв. 5, 2025
Transforming plastics into single-atom catalysts is a promising strategy for upcycling waste value-added functional materials. Herein, graphene-based catalyst with atomically dispersed FeN
Язык: Английский
Процитировано
8
ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер unknown
Опубликована: Фев. 13, 2025
Язык: Английский
Процитировано
5
ACS Catalysis, Год журнала: 2025, Номер unknown, С. 5339 - 5369
Опубликована: Март 17, 2025
Язык: Английский
Процитировано
4