Single and double transition metal atoms doped graphdiyne for highly efficient electrocatalytic reduction of nitric oxide to ammonia

Wu, Yuting; Lv, Jiarui; Xie, Fengjing; An, RunZhi; Zhang, Jiaojiao; Huang, Hong; Shen, Zhangfeng; Jiang, Lingchang; Xu, Minhong; Yao, Qiufang; Cao, Yongyong

doi:10.1016/j.jcis.2023.11.053

Cited by 14 publications

(6 citation statements)

References 57 publications

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“…[ 37 ] In addition, as shown in Figure S31 (Supporting Information), electronic states of Ir@NiFe‐MOF and NiFe‐MOF were continuously distributed around the Fermi level ( ε f ), and both exhibited zero bandgaps, indicating their metallic characteristics. Notably, the total density of states (DOS) at near the Fermi level in Ir@NiFe‐MOF exceeded that of Ir NPs and NiFe‐MOF, indicating that the heterostructure constructed with Ir NPs and NiFe‐MOF through Ir─O─Ni/Fe bonding exhibited enhanced conductivity compared to either monomer, [ 38 ] consistent with the EIS results. Furthermore, a lower d‐band center ( ε d ) indicates a stronger adsorption ability for the intermediates.…”

Section: Resultssupporting

confidence: 67%

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

Li,

Zhang,

Cao

et al. 2024

Advanced Science

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Creating specific noble metal/metal‐organic framework (MOF) heterojunction nanostructures represents an effective strategy to promote water electrolysis but remains rather challenging. Herein, a heterojunction electrocatalyst is developed by growing Ir nanoparticles on ultrathin NiFe‐MOF nanosheets supported by nickel foam (NF) via a readily accessible solvothermal approach and subsequent redox strategy. Because of the electronic interactions between Ir nanoparticles and NiFe‐MOF nanosheets, the optimized Ir@NiFe‐MOF/NF catalyst exhibits exceptional bifunctional performance for the hydrogen evolution reaction (HER) (η10 = 15 mV, η denotes the overpotential) and oxygen evolution reaction (OER) (η10 = 213 mV) in 1.0 m KOH solution, superior to commercial and recently reported electrocatalysts. Density functional theory calculations are used to further investigate the electronic interactions between Ir nanoparticles and NiFe‐MOF nanosheets, shedding light on the mechanisms behind the enhanced HER and OER performance. This work details a promising approach for the design and development of efficient electrocatalysts for overall water splitting.

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Section: Resultssupporting

confidence: 67%

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

Li,

Zhang,

Cao

et al. 2024

Advanced Science

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“…Therefore, Cu/Ti 3 C 2 O 2 -V 0 and Ni/Ti 3 C 2 O 2 -Ti 1 are identified as the most promising SACs for the NORR with spontaneous NORR and high selectivity to NH 3 . The spontaneous NORR on Cu/Ti 3 C 2 O 2 -V 0 and Ni/Ti 3 C 2 O 2 -Ti 1 surpasses most of the theoretically predicted NORR electrocatalysts, as indicated by a positive value of Δ G max for NORR often predicted in previous reports, such as 0.33 eV on Zr–C 2 N, 0.36 eV on Ti/Mo codoped g -CN, 0.1 eV on Cu-graphdiyne, and 0.11 eV on Cr 1 /HfSi 2 N 4 . Notably, the NORR energy profile on Cu/Ti 3 C 2 O 2 -V 0 in this work is comparable to that of spontaneous NORR on a pure metal Cu (111) surface .…”

supporting

confidence: 62%

“…49 Therefore, the whole reaction of NORR should be easier than N 2 O production to guarantee selectivity to NH 3 . As displayed in Figure 3 and Figure S5, the NORR and N 2 O formation performance on the six systems were verified by constructing the Gibbs free-energy diagrams after screening all the reaction pathways, as illustrated in Figure 2 52 and 0.11 eV on Cr 1 /HfSi 2 N 4 . 53 Notably, the NORR energy profile on Cu/Ti 3 C 2 O 2 -V 0 in this work is comparable to that of spontaneous NORR on a pure metal Cu (111) surface.…”

mentioning

confidence: 84%

From Single Atom to Low-Nuclearity Cluster Immobilized Ti₃C₂T_X MXene for Highly Efficient NO Electroreduction to NH₃

Kong,

Wang,

2024

ACS Materials Lett.

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Single-atom catalysts (SACs) have improved the performance of NO electroreduction to NH 3 (NORR) to a high level. However, the influence of low-nuclearity clusters, which exist in SACs as well, on the catalytic performance is always overlooked. Herein, via density functional theory, we not only designed 9 single TMs, namely, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, and Cu, anchored on three Tiand Ti 3 C 2 O 2 -Ti 1 ) as catalysts for NORR but also further evaluated the impact of low-nuclearity clusters on optimal SAC. Our results identified Cu/Ti 3 C 2 O 2 -V 0 and Ni/Ti 3 C 2 O 2 -Ti 1 as promising SACs for the ultrahigh performance of NORR. Furthermore, NORR activity on both SACs diminished with the formation of the low-nuclearity cluster, especially for Ni clusters on Ti 3 C 2 O 2 -Ti 1 . From Ni single atoms to Ni clusters, the projected density of states increases significantly near the Fermi level, leading to stronger interactions between Ni clusters and reaction intermediates, thereby hindering hydrogenation steps and greatly slowing down the NORR on the Ni cluster. Meanwhile, a pH-dependent catalytic activity analysis revealed that the rate-determining step changed as the pH increased on Ni/Ti 3 C 2 O 2 -Ti 1 , and an acidic environment facilitates the effective NOto-NH 3 conversion on Cu/Ti 3 C 2 O 2 -V 0 . Therefore, this work not only predicts the highly efficient NORR catalyst but also reveals the weakening mechanism of low-nuclearity clusters that would guide future experimental research on SACs and metal clusters for NORR.

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“…Following the unveiling of single-atom catalysts (SACs) in 2011, with the exemplar of a single Pt atom doped onto iron oxide showcasing extraordinary catalytic prowess in CO oxidation . This breakthrough has garnered widespread attention and has been applied in various fields of electrocatalysis, including nitrogen reduction reaction (NRR), , hydrogen evolution reaction (HER), , and nitric oxide reduction reaction (NORR). − SACs characterized by their distinct single-atom coordination environments with unsaturated features facilitate enhanced adsorption of reactants and intermediates, thereby delivering heightened activity, selectivity, and optimal atom utilization. A notable example includes the deployment of single copper atoms on carbon nanotubes, which demonstrate exceptional catalytic efficiency in CO 2 RR .…”

Section: Introductionmentioning

confidence: 99%

Screening of Transition Metal Supported on Black Phosphorus as Electrocatalysts for CO₂ Reduction

Zhong,

Yue,

Zhang

et al. 2024

Inorg. Chem.

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The electrocatalytic CO 2 reduction (CO 2 RR) is an effective and economical strategy to eliminate CO 2 through conversion into value-added chemicals and fuels. However, exploring and screening suitable 2D material-based single-atom catalysts (SACs) for CO 2 reduction are still a great challenge. In this study, 27 (3d, 4d, and 5d, except Tc and Hg) transition metal (TM) atom-doped black phosphorus (TM@BP) electrocatalysts were systematically investigated for CO 2 RR by density functional theory calculations. According to the stability of SACs and their effectiveness in activating the CO 2 molecule, three promising catalysts, Zr@BP, Nb@BP, and Ru@BP, were successfully screened out, exhibiting outstanding catalytic activity for the production of carbon monoxide (CO), methyl alcohol (CH 3 OH), and methane (CH 4 ) with limiting potentials of −0.79, −0.49, and −0.60 V, respectively. A catalytic relationship between the d-band centers of SACs and the limiting potential of CO 2 RR was used to estimate the catalytic activity of catalysts. Furthermore, Nb@BP has high selectivity for CO 2 RR to CH 3 OH compared to H 2 formation, while the hydrogen evolution reaction significantly impacts the synthesis of CO and CH 4 on Zr@BP and Ru@BP. Nitrogen atom doping in BP is beneficial for enhancing the selectivity of CO 2 RR, but it is detrimental to the activity of CO 2 RR. This study offers theoretical guidance for synthesizing highly efficient CO 2 RR electrocatalysts and further enhances structural modulation methods for layered 2D materials.

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Single and double transition metal atoms doped graphdiyne for highly efficient electrocatalytic reduction of nitric oxide to ammonia

Cited by 14 publications

References 57 publications

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

From Single Atom to Low-Nuclearity Cluster Immobilized Ti₃C₂T_X MXene for Highly Efficient NO Electroreduction to NH₃

Screening of Transition Metal Supported on Black Phosphorus as Electrocatalysts for CO₂ Reduction

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Single and double transition metal atoms doped graphdiyne for highly efficient electrocatalytic reduction of nitric oxide to ammonia

Cited by 14 publications

References 57 publications

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

From Single Atom to Low-Nuclearity Cluster Immobilized Ti3C2TX MXene for Highly Efficient NO Electroreduction to NH3

Screening of Transition Metal Supported on Black Phosphorus as Electrocatalysts for CO2 Reduction

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Product

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From Single Atom to Low-Nuclearity Cluster Immobilized Ti₃C₂T_X MXene for Highly Efficient NO Electroreduction to NH₃

Screening of Transition Metal Supported on Black Phosphorus as Electrocatalysts for CO₂ Reduction