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  • 1
    Online Resource
    Online Resource
    p ‐Block Bismuth Nanoclusters Sites Activated by Atomically Dispersed Bismuth for Tandem Boosting Electrocatalytic Hydrogen Peroxide Production
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 34 ( 2023-08-21)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 34 ( 2023-08-21)
    Abstract: Constructing electrocatalysts with p ‐block elements is generally considered rather challenging owing to their closed d shells. Here for the first time, we present a p ‐block‐element bismuth‐based (Bi‐based) catalyst with the co‐existence of single‐atomic Bi sites coordinated with oxygen (O) and sulfur (S) atoms and Bi nanoclusters (Bi clu ) (collectively denoted as BiOS SA /Bi clu ) for the highly selective oxygen reduction reaction (ORR) into hydrogen peroxide (H 2 O 2 ). As a result, BiOS SA /Bi clu gives a high H 2 O 2 selectivity of 95 % in rotating ring‐disk electrode, and a large current density of 36 mA cm −2 at 0.15 V vs. RHE, a considerable H 2 O 2 yield of 11.5 mg cm −2 h −1 with high H 2 O 2 Faraday efficiency of ∼90 % at 0.3 V vs. RHE and a long‐term durability of ∼22 h in H‐cell test. Interestingly, the experimental data on site poisoning and theoretical calculations both revealed that, for BiOS SA /Bi clu , the catalytic active sites are on the Bi clusters, which are further activated by the atomically dispersed Bi coordinated with O and S atoms. This work demonstrates a new synergistic tandem strategy for advanced p ‐block‐element Bi catalysts featuring atomic‐level catalytic sites, and the great potential of rational material design for constructing highly active electrocatalysts based on p ‐block metals.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.34
    DOI: 10.1002/anie.202304488
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 2
    Online Resource
    Online Resource
    Atomic-level engineering Fe 1 N 2 O 2 interfacial structure derived from oxygen-abundant metal–organic frameworks to promote electrochemical CO 2 reduction
    Royal Society of Chemistry (RSC) ; 2022
    In:  Energy & Environmental Science Vol. 15, No. 9 ( 2022), p. 3795-3804
    Details
    In: Energy & Environmental Science, Royal Society of Chemistry (RSC), Vol. 15, No. 9 ( 2022), p. 3795-3804
    Abstract: Atomically-precise preparation and atomic-level understanding of the single-atomic active sites with unique coordination structures in electrocatalysts for the CO 2 reduction reaction (CO 2 RR) remain a challenge. Here, we report a strategy of nitrogen (N) source-assisted pyrolysis of an oxygen-abundant MOF precursor (MOF-74) to give uniform, atomically-precise Fe sites, which consist of each Fe central atom coordinated simultaneously with two oxygen (O) atoms and two N atoms, and are anchored on N-doped carbon (thus denoted as Fe 1 N 2 O 2 /NC). By in situ synchrotron X-ray absorption spectroscopy, we have monitored the evolution of coordination structures of Fe atoms (in terms of coordinating atoms and coordination number) along with the increasing pyrolysis temperature. The obtained electrocatalyst exhibits a high selectivity with the faradaic efficiency for CO above 95% over a wide potential range from −0.4 to −0.8 V (in particular, 99.7% at −0.5 V), and a robust durability. Theoretical simulations demonstrate that the ratio of the numbers of coordinating N and O around Fe is very important for regulating the catalytic activity and selectivity of CO 2 -to-CO conversion. Compared with mono-coordinated Fe sites, the N 2 O 2 -coordinated Fe sites have lower free energy change for the steps of COOH* formation and CO desorption, resulting in accelerated reaction kinetics and elevated catalytic activity. This work provides an efficient strategy to prepare well-defined single-atomic active sites via high-precision manipulation of coordinating atoms to boost the catalytic performances for the CO 2 RR.
    Type of Medium: Online Resource
    ISSN: 1754-5692 , 1754-5706
    URL: Article
    DOI: 10.1039/D2EE00878E
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2022
    detail.hit.zdb_id: 2439879-2
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  • 3
    Online Resource
    Online Resource
    Tailoring the selectivity and activity of oxygen reduction by regulating the coordination environments of carbon-supported atomically dispersed metal sites
    Royal Society of Chemistry (RSC) ; 2022
    In:  Journal of Materials Chemistry A Vol. 10, No. 35 ( 2022), p. 17948-17967
    Details
    In: Journal of Materials Chemistry A, Royal Society of Chemistry (RSC), Vol. 10, No. 35 ( 2022), p. 17948-17967
    Abstract: The oxygen reduction reaction (ORR) is an important half reaction in fuel cells and metal–air batteries as well as in the cost-effective electrosynthesis of H 2 O 2 . However, the issues of low selectivity and activity still call for solutions. The key to rationally optimizing the activity and selectivity of electrocatalysts for the ORR is to control their electronic structures. Carbon-supported atomically dispersed metal sites (C-ADMSs) feature isolated metal atoms with well-defined local coordination structures in a carbon host matrix, in which the coordination bonds, bond lengths and coordination number can be modulated to alter the selectivity/activity for the ORR. Benefiting from their metalloenzyme-like properties, C-ADMSs have been serving as an ideal and adjustable platform to controllably regulate the selectivity and activity for the ORR. Therefore, an in-depth summary of the regulation of coordination structures for the ORR is of great significance and a pressing need. In this review, we focus on the manipulation of the coordination number in the first coordination shell and the coordination atoms in the first, second and even outer coordination shells. Then, we summarize the influences of coordination numbers and coordination atoms in different coordination shells on the selectivity for 2e − ORR and the activity for 4e − ORR, respectively. In addition, we attempt to figure out the general principle of the regulating mechanism between the coordination environment and the catalytic activity/selectivity for the ORR. Finally, we present a brief conclusion, and discuss the challenges and opportunities with respect to the active microenvironment of central metals in C-ADMSs for the ORR.
    Type of Medium: Online Resource
    ISSN: 2050-7488 , 2050-7496
    URL: Article
    DOI: 10.1039/D2TA05110A
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2022
    detail.hit.zdb_id: 2702232-8
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  • 4
    Online Resource
    Online Resource
    Multi-interfacial charge polarization for enhancing the hydrogen evolution reaction
    Royal Society of Chemistry (RSC) ; 2023
    In:  Catalysis Science & Technology Vol. 13, No. 14 ( 2023), p. 4107-4116
    Details
    In: Catalysis Science & Technology, Royal Society of Chemistry (RSC), Vol. 13, No. 14 ( 2023), p. 4107-4116
    Abstract: For metal–carbon shell catalysts of the hydrogen evolution reaction (HER), owing to the diversity of the inner metal phases and the adjustability of the outer carbon structure, the structure of the active sites is still puzzling. Here, with the guidance of density functional theory (DFT) calculations, verification of experimental results and operando X-ray absorption spectroscopy, we found that the multi-interfacial charge polarization around Mo atoms in MoP induced by S on MoS 2 and N on adjacent NC layers in carbon defect locations of three phase interfaces could improve the adsorption/desorption behavior of H intermediates and accelerate the dissociative adsorption process of H 2 O molecules, which then exhibited distinct catalytic activities for the HER in both acidic (10.0 mA cm −2 at η = 120 mV) and alkaline media (10.0 mA cm −2 at η = 80 mV) and outstanding durability. This work offers atom-level insights into the active sites of metal–carbon shell catalysts, contributing to the rational design of efficient HER catalysts. Under the guidance of theoretical calculations, the present paper provides a new catalyst with novel inner metal cores of MoP nanoparticles (NPs) coupled with ultrafine MoS 2 nanosheets encapsulated with NC shells. A combination of theoretical calculations and electrochemical analysis uncovers that the multi-interfacial charge polarization of MoP, MoS 2 and NC in carbon defect locations could improve the HER performance in both acidic and alkaline media.
    Type of Medium: Online Resource
    ISSN: 2044-4753 , 2044-4761
    URL: Article
    DOI: 10.1039/D3CY00323J
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2023
    detail.hit.zdb_id: 2595090-3
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  • 5
    Online Resource
    Online Resource
    p ‐Block Bismuth Nanoclusters Sites Activated by Atomically Dispersed Bismuth for Tandem Boosting Electrocatalytic Hydrogen Peroxide Production
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 34 ( 2023-08-21)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 34 ( 2023-08-21)
    Abstract: Constructing electrocatalysts with p ‐block elements is generally considered rather challenging owing to their closed d shells. Here for the first time, we present a p ‐block‐element bismuth‐based (Bi‐based) catalyst with the co‐existence of single‐atomic Bi sites coordinated with oxygen (O) and sulfur (S) atoms and Bi nanoclusters (Bi clu ) (collectively denoted as BiOS SA /Bi clu ) for the highly selective oxygen reduction reaction (ORR) into hydrogen peroxide (H 2 O 2 ). As a result, BiOS SA /Bi clu gives a high H 2 O 2 selectivity of 95 % in rotating ring‐disk electrode, and a large current density of 36 mA cm −2 at 0.15 V vs. RHE, a considerable H 2 O 2 yield of 11.5 mg cm −2 h −1 with high H 2 O 2 Faraday efficiency of ~90 % at 0.3 V vs. RHE and a long‐term durability of ~22 h in H‐cell test. Interestingly, the experimental data on site poisoning and theoretical calculations both revealed that, for BiOS SA /Bi clu , the catalytic active sites are on the Bi clusters, which are further activated by the atomically dispersed Bi coordinated with O and S atoms. This work demonstrates a new synergistic tandem strategy for advanced p ‐block‐element Bi catalysts featuring atomic‐level catalytic sites, and the great potential of rational material design for constructing highly active electrocatalysts based on p ‐block metals.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.34
    DOI: 10.1002/ange.202304488
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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  • 6
    Online Resource
    Online Resource
    Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO2 Electroreduction
    American Chemical Society (ACS) ; 2023
    In:  ACS Nano Vol. 17, No. 5 ( 2023-03-14), p. 4619-4628
    Details
    In: ACS Nano, American Chemical Society (ACS), Vol. 17, No. 5 ( 2023-03-14), p. 4619-4628
    Type of Medium: Online Resource
    ISSN: 1936-0851 , 1936-086X
    URL: Article
    URL: Article
    DOI: 10.1021/acsnano.2c10701
    DOI: 10.1021/acsnano.2c10701.s001
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2023
    detail.hit.zdb_id: 2383064-5
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