Nanocarbon Catalysts: Recent Understanding Regarding the Active Sites

Zhang, Luhua; Shi, Yumeng; Wang, Ye; Shiju, N. Raveendran

doi:10.1002/advs.201902126

Cited by 122 publications

(84 citation statements)

References 196 publications

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“…To this end, coupling with one or more materials to construct PCN-based heterojunctions can enlarge the interfacial junction to promote charge separation and extend the light absorption range to the visible region. [7,[11][12][13][14][15][16] The aligned built-in electric field at the interfacial junction will result in effective charge separation and high PHE performance.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Wang

Chen

et al. 2020

Adv Funct Materials

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Efficient solar-to-hydrogen (STH) energy conversion under ambient conditions (room temperature and atmospheric pressure) is important for pursuing scalable solar hydrogen generation. Modification of polymeric carbon nitride (PCN) by conjugated polymers has attracted great attention for improving photocatalytic hydrogen evolution (PHE) performance. However, the limited interfacial junction between PCN and conjugated polymers leads to a low density of free charges, resulting in unsatisfactory PHE activity. Herein, three donor-π-acceptor-structured organic molecules (OMs) with different electron-donating units (amino, N,N-diethyl and triphenylamine) and same electron-accepting unit (benzothiadiazole) are designed to modify PCN to enlarge the interfacial junction. The optimized PHE performance under AM 1.5G simulated sunlight and ambient conditions can maintain as high as 4.63 mmol h −1 g −1 (the highest record among all the reported PCN-based photocatalysts to the best of the authors knowledge). The improved performance can be partially attributed to the strong visible light harvesting capability of OMs. Specifically, the triphenylamine unit in the formed type II molecule heterojunctions (MHJ) enables efficient charge separation at the interfacial junction, which prolongs the photogenerated electron lifetime for PHE. The designed MHJ photocatalysts show outstanding PHE performance under ambient conditions, which is highly promising for scalable STH conversion.

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Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Wang

Chen

et al. 2020

Adv Funct Materials

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“…The surface charge and potential analysis along with DFT calculations confirmed a strong correlation between the catalytic activity of active sites and surface charges, providing evidence for those defects can significantly enhance the catalytic activity of ORR and OER [44] . Topological defects and edge defects, two types of the most common line defects of nanocarbon materials, have been widely concerned as active sites of ORR or OER [45] …”

Section: Intrinsic Carbon Defectsmentioning

confidence: 86%

“…[44] Topological defects and edge defects, two types of the most common line defects of nanocarbon materials, have been widely concerned as active sites of ORR or OER. [45]…”

Section: Intrinsic Carbon Defectsmentioning

confidence: 99%

Defect Engineering of Carbon‐based Electrocatalysts for Rechargeable Zinc‐air Batteries

Dong

Zhang

et al. 2020

Chemistry An Asian Journal

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Rechargeable zinc-air batteries (ZABs) are considered as one of the most promising electrochemical energy devices due to their various unique advantages. Oxygen electrocatalysis, involving the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), determines the overall performance of zinc-air batteries. Therefore, the development of highly efficient bifunctional ORR/OER catalysts is critical for the large-scale application of ZABs. Carbonbased nanomaterials have been widely reported to be efficient electrocatalysts toward both ORR and OER. The enhanced activity of these electrocatalysts are usually attributed to different doping defects, synergistic effects and even the intrinsic carbon defects. Herein, an overview of the defect engineering in carbon-based electrocatalysts for ORR and OER is provided. The different types of intrinsic carbon defects and strategies for the generation of other defects in carbon-based electrocatalysts are presented. The interaction of heteroatoms doped carbon and transition metals (TMs) is also explored. In the end, the existing challenges and future perspectives on defect engineering are discussed.

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“…Graphene has received enormous interest due to its two‐dimensional (2D) structure, excellence electrical, thermal, optical and mechanical properties [17] . Noting that pristine graphene is chemically inert and is not active for heterogeneous catalysis, [18] thus the surface modifications with heteroatoms and creating defects as the efficient strategies to enhance the surface active [19–21] . Similar as the graphene, graphenylene as a novel sp 2 ‐hybridized carbon network is composed of hexagonal units (C 6 rings) and square units (C 4 rings) [22] and has periodic pores with a diameter of 3.2 Å.…”

Section: Introductionmentioning

confidence: 99%

Comparative Study of NO and CO Oxidation Reactions on Single‐Atom Catalysts Anchored Graphene‐like Monolayer

et al. 2021

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Noble metal single‐atom catalysts (NM‐SACs) anchored at novel graphene‐like supports has attracted enormous interests. Gas sensitivity, catalytic activity, and d‐band centers of single NM (Pt and Pd) atoms at graphenylene (graphenylene‐NM) are investigated using first‐principle calculations. The adsorption geometries of gas reactants on graphenylene‐NM sheets are analyzed. It is found that the adsorption energies of reactant species on graphenylene‐Pt are larger than those on graphenylene‐Pd, because the d‐band center of the Pt atom is closeser to the Fermi level. The NO and CO oxidation reactions on graphenylene‐NM are investigated via four catalytic mechanisms, including Langmuir‐Hinshelwood (LH), Eley‐Rideal (ER), New ER (NER), and termolecular ER (TER). The results show that the NO and CO oxidations via LH and TER mechanisms can occur owing to the relatively small energy barriers. Moreover, the interaction of 2NO+2CO via ER mechanism is the energetically more favorable reaction. Although the NO oxidation via the NER mechanism has rather low energy barriers, the reaction is unlikely to occur due to the low adsorption energy of O2 compared with CO and NO. This research may provide guidance for exploring the catalytic performance of SACs on graphene‐like materials to remove toxic gas molecules.

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Nanocarbon Catalysts: Recent Understanding Regarding the Active Sites

Cited by 122 publications

References 196 publications

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Defect Engineering of Carbon‐based Electrocatalysts for Rechargeable Zinc‐air Batteries

Comparative Study of NO and CO Oxidation Reactions on Single‐Atom Catalysts Anchored Graphene‐like Monolayer

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