Tunable Carbon Surface from Mono- to Multi-Metallic Single Atoms

Herein, we develop a non-selective charge compensation strategy to prepare multi-single-atom doped carbon (MSAC) in which a sodium p-toluenesulfonate (PTS-Na) doped polypyrrole (S-PPy) polymer is designed to anchor discretionary mixtures of multiple metal cations, including iron (Fe3+), cobalt (Co3+), ruthenium (Ru3+), palladium (Pd2+), indium (In3+), iridium (Ir2+), and platinum (Pt2+) . As illustrated in Figure 1, the carbon surface can be tuned with different level of compositional complexities, including unary Pt1@NC, binary (MSAC-2, (PtFe)1@NC), ternary (MSAC-3, (PtFeIr)1@NC), quaternary (MSAC-4, (PtFeIrRu)1@NC), quinary (MSAC-5, (PtFeIrRuCo)1@NC), senary (MSAC-6, (PtFeIrRuCoPd)1@NC), and septenary (MSAC-7, (PtFeIrRuCoPdIn)1@NC) samples. The structural evolution of carbon surface dictates the activities of both ORR and HER. The senary MSAC-6 achieves the ORR mass activity of 18.1 A·mgmetal-1 at 0.9 V (Vs reversible hydrogen electrode (RHE)) over 30K cycles, which is 164 times higher than that of commercial Pt/C. The quaternary MSAC-4 presented a comparable HER catalytic capability with that of Pt/C. These results indicate that the highly complexed carbon surface can enhance its ability over general electrochemical catalytic reactions. The mechanisms regarding of the ORR and HER activities of the alternated carbon surface are also theoretically and experimentally investigated in this work, showing that the synergistic effects amongst the co-doped atoms can activate or inactivate certain single-atom sites.

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Ligand-coordinated Ir single-atom catalysts stabilized on oxide supports for ethylene hydrogenation and their evolution under a reductive atmosphere

Catalysis Science & Technology ◽

10.1039/d0cy01132k ◽

2021 ◽

Author(s):

Linxiao Chen ◽

Iyad S. Ali ◽

George E. Sterbinsky ◽

Xuemei Zhou ◽

Eman Wasim ◽

...

Keyword(s):

Structural Evolution ◽

Single Atom ◽

Ethylene Hydrogenation ◽

Oxide Supports ◽

Single Atoms ◽

Reducing Atmosphere ◽

Reductive Atmosphere

Effective, stable, durable, and tunable Ir-ligand single-atom catalysts for ethylene hydrogenation, studied in situ for structural evolution of Ir single-atoms under a reducing atmosphere.

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Single–atom manganese and nitrogen co-doped graphene as low-cost catalysts for the efficient CO oxidation at room temperature

Applied Surface Science ◽

10.1016/j.apsusc.2020.147809 ◽

2021 ◽

Vol 536 ◽

pp. 147809

Author(s):

Mingming Luo ◽

Zhao Liang ◽

Chao Liu ◽

Xiaopeng Qi ◽

Mingwei Chen ◽

...

Keyword(s):

Co Oxidation ◽

Room Temperature ◽

Low Cost ◽

Single Atom ◽

Doped Graphene ◽

Co Doped

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Improving peroxymonosulfate activation by copper ion-saturated adsorbent-based single atom catalysts for the degradation of organic contaminants: electron-transfer mechanism and the key role of Cu single atoms

Journal of Materials Chemistry A ◽

10.1039/d1ta02237g ◽

2021 ◽

Author(s):

Jingwen Pan ◽

Baoyu Gao ◽

Pijun Duan ◽

Kangying Guo ◽

Muhammad Akram ◽

...

Keyword(s):

Electron Transfer ◽

Organic Contaminants ◽

High Salinity ◽

Copper Ion ◽

Single Atom ◽

Electron Transfer Mechanism ◽

Persulfate Oxidation ◽

Single Atoms ◽

Oxidation Technology

Nonradical pathway-based persulfate oxidation technology is considered to be a promising method for high-salinity organic wastewater treatment.

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Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst

ACS Catalysis ◽

10.1021/acscatal.0c05599 ◽

2021 ◽

Vol 11 (4) ◽

pp. 1952-1961

Author(s):

Junhong Fu ◽

Jinhu Dong ◽

Rui Si ◽

Keju Sun ◽

Junying Zhang ◽

...

Keyword(s):

Synergistic Effects ◽

Single Atom

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Active site engineering of atomically dispersed transition metal-heteroatom-carbon catalysts for oxygen reduction

Chemical Communications ◽

10.1039/d1cc03076k ◽

2021 ◽

Author(s):

Jiawei Zhu ◽

Shichun Mu

Keyword(s):

Transition Metal ◽

Oxygen Reduction ◽

Active Site ◽

Catalytic Reactions ◽

Single Atom ◽

Carbon Catalysts

Owing to the advantage of atomic utilization, the single-atom catalyst has attracted much attention and been employed in multifarious catalytic reactions. Their definite site configuration is favorable for exploring the...

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Synergy of Single Atoms Pd and Oxygen Vacancies on In2O3 for Highly Selective C1 Oxygenates Production from Methane under Visible Light

10.21203/rs.3.rs-942037/v1 ◽

2021 ◽

Author(s):

Lei Luo ◽

Lei Fu ◽

Huifen Liu ◽

Youxun Xu ◽

Jialiang Xing ◽

...

Keyword(s):

Oxygen Vacancies ◽

Single Atom ◽

Electron Transfer Pathway ◽

Mild Conditions ◽

Single Atoms ◽

Primary Products ◽

Critical Issues ◽

Regulation Of Activity ◽

Visible Irradiation ◽

Dft Modelling

Abstract Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues on both conversion and selectivity. Herein, under visible irradiation (420 nm), the synergy of palladium (Pd) atom cocatalyst and oxygen vacancies (OVs) on In2O3 nanorods enabled superior photocatalytic CH4 activation by O2. The optimised catalyst reached ca. 100 µmol·h− 1 of C1 oxygenates, with a selectivity of primary products (CH3OH and CH3OOH) up to 82.5 %. Mechanism investigation elucidated that such superior photocatalysis was induced by the dedicated function of Pd single atoms and oxygen vacancies on boosting hole and electron transfer pathway, respectively. O2 was proven to be the only oxygen source for CH3OH production, while H2O acted as the promoter for efficient CH4 activation through ·OH production and facilitated product desorption as indicated by DFT modelling. This work thus provides new understandings on simultaneous regulation of activity and selectivity by the significant synergy of single atom cocatalysts and oxygen vacancies.

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Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions

Advanced Science ◽

10.1002/advs.201801471 ◽

2018 ◽

Vol 6 (3) ◽

pp. 1801471 ◽

Cited By ~ 12

Author(s):

Hongliang Li ◽

Menglin Wang ◽

Laihao Luo ◽

Jie Zeng

Keyword(s):

Catalytic Reactions ◽

Single Atom ◽

Dynamic Evolution

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Interfacial-confined coordination to single-atom nanotherapeutics

Nature Communications ◽

10.1038/s41467-021-27640-7 ◽

2022 ◽

Vol 13 (1) ◽

Author(s):

Limei Qin ◽

Jie Gan ◽

Dechao Niu ◽

Yueqiang Cao ◽

Xuezhi Duan ◽

...

Keyword(s):

Therapeutic Strategy ◽

Single Atom ◽

Oxygen Species ◽

High Quality ◽

Efficient Energy ◽

Coordination Strategy ◽

Single Atoms ◽

Highly Active ◽

Narrow Bandgap ◽

Catalytic Sites

AbstractPursuing and developing effective methodologies to construct highly active catalytic sites to maximize the atomic and energy efficiency by material engineering are attractive. Relative to the tremendous researches of carbon-based single atom systems, the construction of bio-applicable single atom materials is still in its infancy. Herein, we propose a facile and general interfacial-confined coordination strategy to construct high-quality single-atom nanotherapeutic agent with Fe single atoms being anchored on defective carbon dots confined in a biocompatible mesoporous silica nanoreactor. Furthermore, the efficient energy conversion capability of silica-based Fe single atoms system has been demonstrated on the basis of the exogenous physical photo irradiation and endogenous biochemical reactive oxygen species stimulus in the confined mesoporous network. More importantly, the highest photothermal conversion efficiency with the mechanism of increased electron density and narrow bandgap of this single atom structure in defective carbon was proposed by the theoretical DFT calculations. The present methodology provides a scientific paradigm to design and develop versatile single atom nanotherapeutics with adjustable metal components and tune the corresponding reactions for safe and efficient tumor therapeutic strategy.

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Intermetallic Platinum Alloy Nanoparticles and Single Atoms Hybrid Electrocatalysts for Proton Exchange Membrane Fuel Cells

10.21203/rs.3.rs-685784/v1 ◽

2021 ◽

Author(s):

Minhua Shao ◽

Fei Xiao ◽

Qi Wang ◽

Gui-Liang Xu ◽

Xueping Qin ◽

...

Keyword(s):

Fuel Cell ◽

Active Sites ◽

Proton Exchange Membrane ◽

Synergistic Effects ◽

Reduction Reaction ◽

Proton Exchange ◽

Alloy Nanoparticles ◽

Single Atoms ◽

Low Pt Loading ◽

Exchange Membrane

Abstract Proton exchange membrane fuel cell converts hydrogen and oxygen into electricity with zero emission1. The high cost and low durability of Pt-based electrocatalysts for oxygen reduction reaction hinder its wide applications2,3. The development of non-precious metal electrocatalysts also reaches the bottleneck because of the low activity and durability4,5. Here we rationally design a hybrid electrocatalyst consisting of atomically dispersed Pt and Fe single atoms and intermetallic PtFe alloy nanoparticles. The Pt mass activity of the hybrid catalyst is 3.5 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with an ultra-low Pt loading in the cathode (0.015 mgPt cm-2) shows unprecedented durability, with 93.6% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for at least 206 h. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.

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