Precisely Tuning the Number of Fe Atoms in Clusters on N-Doped Carbon toward Acidic Oxygen Reduction Reaction

Ye, Wei; Chen, Shuangming; Lin, Yue; Yang, Li; Chen, Sijia; Zheng, Xusheng; Qi, Zeming; Wang, Chengming; Long, Ran; Chen, Meng; Zhu, Junfa; Gao, Peng; Li, Song; Jiang, Jun; Xiong, Yujie

doi:10.1016/j.chempr.2019.07.020

Cited by 400 publications

(359 citation statements)

References 52 publications

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“…Chen and co‐workers also discovered that the single Fe atoms can be coordinated with five N atoms, which modulated the interaction strength of oxygen on Fe ions and further enhanced the ORR activity . Besides, the Fe dimers anchored on N‐doped carbon also showed excellent acidic ORR activity with a half‐wave potential of 0.78 V versus RHE and remarkable stability with only −20 mV shift after 20 000 cycles in 0.5 m H 2 SO 4 electrolyte …”

Section: Structure and Catalytic Activity: Bonding And Coordination Cmentioning

confidence: 97%

Heterogeneous Single Atom Electrocatalysis, Where “Singles” Are “Married”

Zang

Kou

Pennycook

et al. 2020

Advanced Energy Materials

128

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There is an intensive search for heterogeneous single atom catalysts (SACs) of high activity, efficiency, durability, and selectivity for a wide variety of electrocatalytic conversion and chemical reactions, such as the hydrogen evolution reaction (HER), oxygen evolution/reduction reaction (OER and ORR), CO2 reduction reaction (CO2 RR), and nitrogen reduction reaction (NRR). With the downsizing from nanoparticles and clusters to single atoms, there are steady changes in the bond and coordination environment for each and every atom involved. Indeed, the single atoms in these electrocatalysts are not “singles”; they are “married” to the supporting surfaces, and their performance is controlled by the bonding and coordination with the substrate surfaces. Herein, an overview is presented on the brief history leading to the rapid development of SACs and their current status, by focusing on their synthesis, control of composition, strategies to realize single atoms with the desired bonds and coordination, and targeted performance in selected reactions. Their applications in the selected spectrum of energy conversion and chemical reactions are discussed, in relation to their structures at varying length scales down to the atomic level. A particular emphasis is placed on on‐going research activities, together with the future perspectives and particular challenges for SACs.

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Section: Structure and Catalytic Activity: Bonding And Coordination Cmentioning

confidence: 97%

Heterogeneous Single Atom Electrocatalysis, Where “Singles” Are “Married”

Zang

Kou

Pennycook

et al. 2020

Advanced Energy Materials

128

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“…Moreover, DFT results indicate more electrons can be filled into the unoccupied Pt 5d-like orbitals in Pt 2 /graphene and is weakened the adsorption of both AB and H 2 molecules, thus generating the superior activity. The dual metal sites consisting of homo-metal species have also demonstrated their superiority in ORR, [75] NRR [76] and alkene epoxidation. [77] Additionally, there is great interest in synthesizing the adjacent dual-metal-site catalysts with different metal species, which has been demonstrated to be highly effective for improved catalytic performance, including Co-Pt, [72] Fe-Pt, [78] Co-Fe, [79] Pt-Ru, [80] and Ni-Fe [81] materials.…”

Section: Synergy Of Neighboring Single Metal Atomsmentioning

confidence: 99%

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Liu

Ding

et al. 2020

Advanced Energy Materials

Self Cite

218

141

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Single atom catalysts (SACs) that integrate the merits of homogeneous and heterogeneous catalysts have been attracting considerable attention in recent years. The individual metal atoms of SACs can be stabilized on supports through various unsaturated chemical sites or space confinement for achieving the maximized atom utilization efficiency. Aside from the development of strategies for preparing high loading and high purity SACs, another key challenge in this field is precisely manipulating the geometric and electronic structure of catalytically active single metal sites, thus rendering the catalysts exceptionally reactive, selective, and stabile compared to their bulk counterparts. This review summarizes recent advancements in SACs for heterogeneous catalysis from the perspective of local structural regulation and the synergistic coupling effect between metal species and supports. Special emphasis is placed on the elucidation of the catalytic structure‐performance relationship in terms of coordination environment, valence state and metal‐support interactions by advanced characterization and theoretical studies. Select in situ or operando characterization techniques for tracking the SACs’ structure evolution under realistic conditions are highlighted. Finally, the challenges and opportunities are discussed to offer insight into the rational design of more intriguing SACs with high activity and distinct chemoselectivity.

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“…Several candidate systems including Sc2, Ti2, Cr2, Mn2 and Fe2 dimers on the 6N-V6 monolayer have adsorption energies of −3.71 ~ −0.48 eV for fixation of two CO2 molecules (Figure 3 and Figure S3), while the other metal dimers are only able to bind one CO2 molecule. Considering that Fe is an earthabundant element and dispersed Fe atoms and dimers can be readily obtained in the experiment (Ye et al, 2019;Tian et al, 2018), thereafter we explored Fe2 dimer on various nitrogenated 2D holey carbon materials as a representative of dual metal centers. and 4N-V2, 5N-V3, and 6N-V4(a) increases with both N content and hole size.…”

Section: As Presented Inmentioning

confidence: 99%

“…Furthermore, homonuclear and heteronuclear dimers of transition metal immobilized in carbon based nanostructures, such as Fe2 and Fe-Co on nitrogenated graphitic carbon materials, Fe-Ni on N-doped graphene, and Pt-Ru on g-C3N4, have been synthesized in the laboratory (Ye et al, 2019;Wang et al, 2017;Zhou et al, 2019). This opens up the windows for a broader range of chemical processes that require dual reaction centers either with enhanced activity or carrying different functionalities simultaneously.…”

Section: Introductionmentioning

confidence: 99%

Selective C−C Coupling by Spatially Confined Dimeric Metal Centers

Zhao

2020

iScience

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Direct conversion of carbon dioxide (CO2) to high-energy fuels and high-value chemicals is a fascinating sustainable strategy. For most of the current electrocatalysts for CO2 reduction, however, multi-carbon products are inhibited by large overpotentials and low selectivity. For practical applications, there remains a big gap of knowledge in proper manipulation of the C−C coupling process. Herein, we exploit dispersed 3d transition metal dimers as spatially confined dual reaction centers for selective reduction of CO2 to liquid fuels. Various nitrogenated holey carbon monolayers are shown to be promising templates to stabilize these metal dimers and dictate their electronic structures, allowing precise control of the catalytic activity and product selectivity. By comprehensive first-principles calculations, we screen the suitable transition metal dimers that universally have high activity for ethanol (C2H5OH). Furthermore, remarkable selectivity for C2H5OH against other C1 and C2 products is found for Fe2 dimer anchored on C2N monolayer. The correlation between the activity and d band center of the supported metal dimer as well as the role of electronic coupling between the metal dimer and the carbon substrates are thoroughly elucidated.

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Precisely Tuning the Number of Fe Atoms in Clusters on N-Doped Carbon toward Acidic Oxygen Reduction Reaction

Cited by 400 publications

References 52 publications

Heterogeneous Single Atom Electrocatalysis, Where “Singles” Are “Married”

Heterogeneous Single Atom Electrocatalysis, Where “Singles” Are “Married”

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Selective C−C Coupling by Spatially Confined Dimeric Metal Centers

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