Continuous Homogeneous Catalytic Oxidation of C–H Bonds by Metal-Free Carbon Dots with a Poly(ascorbic acid) Structure

Wang, Xiao; Chen, Shaoang; Ma, Yurong; Zhang, Tianyang; Zhao, Yajie; He, Tiwei; Huang, Hui; Zhang, Shitong; Rong, Junfeng; Shi, Chunfeng; Tang, K.; Liu, Yang; Kang, Zhenhui

doi:10.1021/acsami.2c03627

Cited by 13 publications

(7 citation statements)

References 42 publications

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“…For example, with the assistance of ML, Wu et al successfully synthesized CDs with enhanced quantum yields (Figure A) . Recently, we accurately predicted by ML and fabricated metal-free CDs with an ascorbic acid-based polymer-like structure (Figure B,C), which could unprecedentedly serve as homogeneous catalysts for oxidation of C–H bonds and deliver high selectivity from cyclohexane to adipic acid . Moreover, for the first time, we successfully confirmed that ML could be utilized to realize the design, manufacturing, and performance adjustment of light emitting devices (Figure D) …”

Section: New Methods Gaining Deep Insightssupporting

confidence: 57%

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Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

2022

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Conspectus As a new kind of carbon based functional material, carbon dots (CDs) have sparked much interest in recent years. The tunable structure, composition, and morphology of CDs unlocks opportunities to enable diversity in their photoelectrochemical properties, and thus they show great potential in various applications such as biology, catalysis, sensors, and energy storage. Nevertheless, the related understanding of CDs is insufficient at present due to their inherent complexity of microstructure, which involves the intersection of high polymer, bulk carbon, and quantum dot (QD). A good understanding of the underlying mechanism behind the properties of CDs is still a formidable challenge, requiring the integration of robust knowledge from organic chemistry, materials science, and solid state physics. Within this context, discovering more appealing properties, elucidating fundamental factors that affect the properties and proposing effective engineering strategies that can realize specific functions for CDs are now highly pursued by researchers. At the beginning of this Account, the main features of CDs are introduced, where not only the basic structural, compositional and morphological characteristics but also the rich photoelectrochemical properties are elucidated, among which the band gap, chirality, photoinduced potential, and electron sink effect are particularly emphasized. Furthermore, new analysis techniques including transient photoinduced current (TPC), transient photoinduced voltage (TPV), and machine learning (ML) to reveal the unique properties of CDs are described. Then, several appealing strategies that aim to rationally tailor CDs for oriented applications are highlighted. These regulation strategies are morphology modulation (e.g., developing CDs with new geometrical configuration, controlling the particle size), phase engineering (e.g., altering the phase crystallinity, introducing the foreign atoms), surface functionalization (e.g., grafting various types of functional groups), and interfacial tuning (e.g., building CD-based nanohybrids with well-defined interfaces). Although the fundamental investigation of CDs is relatively undeveloped because of their complexity, this does not hinder their wide application. At the same time, exploring the extensive applications of CDs will promote their in-depth understanding. Finally, the chances for building a CD-centered blueprint for sustainable society are explored and challenges for future research in the field of CDs are proposed as follows: (i) the controllable synthesis of CDs with uniform size; (ii) search for novel CDs with unique structure, morphology, or composition; (iii) quantitative understanding of the property of CDs; (iv) performance enhancement by external forces such as magnetism or heat injection; (v) construction of the dual carbon concept; (vi) further research on different photocatalytic applications. On the whole, this Account may provide meaningful references for the understanding of the microstructure–property correlation as w...

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Section: New Methods Gaining Deep Insightssupporting

confidence: 57%

“…(B) Design framework for the guided synthesis of CDs on homogeneous cyclohexane oxidation based on ML; (C) selectivity and conversion to oxidation products of the catalytic oxidation of nine hydrocarbon molecules using CDs as catalysts . Reproduced with permission from ref . Copyright 2022 American Chemical Society.…”

Section: New Methods Gaining Deep Insightsmentioning

confidence: 99%

Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

2022

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“…Other sulfide compounds incorporated with the metals of Mo, [ 72–74 ] Ni, [ 75,76 ] Zn, [ 77–79 ] and Fe [ 80–82 ] also exhibit great prospect in mediating LPS adsorption and precipitation. Cao et al.…”

Section: Mediation Of Electrolyte–substrate Interfacementioning

confidence: 99%

Interface Engineering Toward Expedited Li₂S Deposition in Lithium–Sulfur Batteries: A Critical Review

Sun

Liu

et al. 2023

Advanced Materials

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Lithium–sulfur batteries (LSBs) with superior energy density are among the most promising candidates of next‐generation energy storage techniques. As the key step contributing to 75% of the overall capacity, Li2S deposition remains a formidable challenge for LSBs applications because of its sluggish kinetics. The severe kinetic issue originates from the huge interfacial impedances, indicative of the interface‐dominated nature of Li2S deposition. Accordingly, increasing efforts have been devoted to interface engineering for efficient Li2S deposition, which has attained inspiring success to date. However, a systematic overview and in‐depth understanding of this critical field are still absent. In this review, the principles of interface‐controlled Li2S precipitation are presented, clarifying the pivotal roles of electrolyte–substrate and electrolyte–Li2S interfaces in regulating Li2S depositing behavior. For the optimization of the electrolyte–substrate interface, efforts on the design of substrates including metal compounds, functionalized carbons, and organic compounds are systematically summarized. Regarding the regulation of electrolyte–Li2S interface, the progress of applying polysulfides catholytes, redox mediators, and high‐donicity/polarity electrolytes is overviewed in detail. Finally, the challenges and possible solutions aiming at optimizing Li2S deposition are given for further development of practical LSBs. This review would inspire more insightful works and, more importantly, may enlighten other electrochemical areas concerning heterogeneous deposition processes.

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“…The oxidation of hydrocarbons into value-added chemical products, especially alkanes that are much more difficult to utilize without active functional groups, is of great importance in the chemical industry. − Cyclohexane oxidation is a typical hydrocarbon resource high-value utilization process, and in this process, the oxidation products including cyclohexanol, cyclohexanone (referred to as KA oil), and adipic acid are important organic intermediates for nylon-6 and nylon-66 in the nylon industry. ,− For the details of cyclohexane oxidation, the widely accepted oxidation process of cyclohexane includes the activation of cyclohexane to a cyclohexyl radical, the transition to KA oil, the further oxidation to adipic acid, and the over oxidation to glutaric acid, succinic acid, and other byproducts, as described in Scheme (b). − As a complex radical oxidation reaction, it is a great challenge to activate the C–H bond and to generate active radicals under proper conditions due to the strong and inert C–H bonds, and on the other hand, it is also an important issue to investigate in order to control the oxidation process to realize the production of target products under high selectivity and avoid over oxidations. − …”

Section: Introductionmentioning

confidence: 99%

Roles of Oxygen Vacancies in CeO₂ Nanostructures for Catalytic Aerobic Cyclohexane Oxidation

et al. 2023

ACS Appl. Nano Mater.

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Nanostructured cerium-based catalytic materials have attracted much attention in the field of redox catalysis, due to the excellent active sites exposed on the nanocrystal surface, and herein, the oxygen vacancy (O V ) and the crystal facet effect of typical model nanostructured ceria (Nano-CeO 2 ) were focused and investigated for the catalytic aerobic cyclohexane oxidation. Specifically for the CeO 2 nanocubes with a {100} facet, the CeO 2 nanopolyhedrons with a dominant {111} facet, and the CeO 2 nanorods with a dominant {110} facet, the catalytic roles of the O V and acid sites toward cyclohexane oxidation were systematically investigated. Surface oxygen vacancy (Sur-O V ) and intrinsic oxygen vacancy (Int-O V ), and particularly the active Sur-O V and active Int-O V performing catalytic activity under a working state specific for cyclohexane oxidation, were accurately recognized and distinguished. Furthermore, the activation ability of the O V sites for activating molecular oxygen into active oxygen species (O Active ) was also revealed, and the acid site properties, which include the acidity and the types of acid sites, were probed and quantified. The Nano-CeO 2 with an exposed {100} facet possesses the most active Sur-O V , determining the catalytic activity, and has the strongest activation ability, contributing to a high reaction activity under extremely inert conditions. The Nano-CeO 2 with a {110} dominant facet with the most active Int-O V and abundant acid sites could accelerate further oxidation to adipic acid; the effect of the two key sites was described particularly by the α factor (= Total Acidity × Amount of Active Int-O V ). Finally, the property−performance relationship toward cyclohexane oxidation was speculated based on the Nano-CeO 2 catalytic system.

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Continuous Homogeneous Catalytic Oxidation of C–H Bonds by Metal-Free Carbon Dots with a Poly(ascorbic acid) Structure

Cited by 13 publications

References 42 publications

Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

Interface Engineering Toward Expedited Li₂S Deposition in Lithium–Sulfur Batteries: A Critical Review

Roles of Oxygen Vacancies in CeO₂ Nanostructures for Catalytic Aerobic Cyclohexane Oxidation

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Continuous Homogeneous Catalytic Oxidation of C–H Bonds by Metal-Free Carbon Dots with a Poly(ascorbic acid) Structure

Cited by 13 publications

References 42 publications

Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

Diversity and Tailorability of Photoelectrochemical Properties of Carbon Dots

Interface Engineering Toward Expedited Li2S Deposition in Lithium–Sulfur Batteries: A Critical Review

Roles of Oxygen Vacancies in CeO2 Nanostructures for Catalytic Aerobic Cyclohexane Oxidation

Contact Info

Product

Resources

About

Interface Engineering Toward Expedited Li₂S Deposition in Lithium–Sulfur Batteries: A Critical Review

Roles of Oxygen Vacancies in CeO₂ Nanostructures for Catalytic Aerobic Cyclohexane Oxidation