Isolated single atomic site catalysts have attracted great interest due to their remarkable catalytic properties. Because of high surface energy, atoms are highly mobile and tend form aggregate during synthetic processes. Therefore, it is a significant challenge fabricate isolated with good stability. Herein, gentle method stabilize metal by constructing defects on the supports presented. As proof concept, Au supported defective TiO2 nanosheets prepared discovered that (1) can effectively...

The electrocatalytic activity of transition-metal-based compounds is strongly related to the spin states. However, underlying relationship connecting catalytic remains unclear. Herein, we carried out density functional theory calculations on oxygen reduction reaction (ORR) catalyzed by Fe single-atom supported C2N (C2N–Fe) shed light this relationship. It found that change electronic moments and O2 due molecular-catalyst adsorption scales with amount electron transfer from O2, which promotes...

Integrating single atoms and clusters into one system is a novel strategy to achieve desired catalytic performances. Compared with homogeneous single-atom cluster catalysts, heterogeneous ones combine the merits of different species therefore show greater potential. However, it still challenging construct systems species, underlying mechanism for activity improvement remains unclear. In this work, we developed catalyst (ConIr1/N-C) efficient oxygen evolution. The Ir worked in synergy Co at...

Abstract Developing efficient and economical electrocatalysts for acidic oxygen evolution reaction (OER) is essential proton exchange membrane water electrolyzers (PEMWE). Cobalt oxides are considered promising non-precious OER catalysts due to their high activities. However, the severe dissolution of Co atoms in acid media leads collapse crystal structure, which impedes application PEMWE. Here, we report that introducing acid-resistant Ir single into lattice spinel cobalt can significantly...

Dual-metal-site catalysts (DMSCs) have emerged as a frontier in heterogeneous catalysis, while the underlying relationships connecting their dual-site synergistic effects on catalytic performance remain unclear. Here we present comprehensive first-principles study of O2 activation and CO oxidation series N-coordinated DMSCs. We discovered that N3-coordinated-adjacent dual-metal model has stronger dynamic effects, leading to much higher activity than others investigated. Based this model,...

Modifying the atomic and electronic structure of platinum-based alloy to enhance its activity anti-CO poisoning ability is a vital issue in hydrogen oxidation reaction (HOR). However, role foreign modifier metal underlying ligand effect not fully understood. Here, we propose that single-atom Cu can dynamically modulate d-band center Pt-based for boosting HOR performance. By situ X-ray absorption spectroscopy, our research has identified potential-driven structural rearrangement into...

The catalytic performance of single-atom catalysts was strictly limited by isolated sites. Fabricating high-density single atoms to realize the synergetic interaction in neighbouring could optimize adsorption behaviors reaction intermediates, which exhibited great potential break limitations and deepen mechanistic understanding electrocatalysis. However, behavior governed is particularly elusive has yet be understood. Herein, we revealed that contributes superior for oxygen evolution...

Polarized charges on dual-reactive centers of C₂N-supported single-atom based transition metal ion catalysts promoting HCOOH dehydrogenation.

The remarkable chemical activity of metal single-atom catalysts (SACs) lies in their unique electronic states associated with the low-coordination nature sites. Yet, state manipulation normally requires direct contact other atoms, which inevitably changes environment. Herein, we found by first-principle calculations that a Co SAC for HCOOH dehydrogenation is appreciably enhanced via noncontact single atom promoter. A and Sn/Ge/Pb are anchored same cavity graphitic C2N monolayer....

Polynary single-atom structures can provide synergistic functions based on multiple active sites and reactants, which significantly improve their catalytic performance. However, the structure–activity relationships of these special remain elusive. Here, we report atomically dispersed Fe–Ni dual-metal catalysts anchored N-doped graphene as an efficient catalyst for CO oxidation. The density functional theory (DFT) calculation results show that Ni serves a nucleophilic center adsorption,...

We performed density functional theory (DFT) calculations to investigate the synergized O2 activation and CO oxidation by Ag8 cluster on TiO2(101) support. The excellent catalytic activity of interfacial Ag atoms in dissociation is ascribed positive polarized charges, upshift d-band center, assistance surface Ti5c atoms. then takes place via a two-step mechanism coupled with dissociation: (i) + → CO2 O (ii) CO2. synergistic effect activations reduces energy barrier (Ea) reaction (i),...

The versatile properties of bimetallic nanoparticles greatly expand the range catalyzed chemical reactions. We demonstrate that surface chemistry can be understood and predicted using a simple adsorbate-surface interaction descriptor relates charge polarization to reactivity. Our density functional theory studies O2 activation CO oxidation by Au7-Cu1 supported on TiO2(101) generated oxidized Cu atom (CuO x) efficiently inhibit aggregation active sites. Moreover, because strong dipole-dipole...

Abstract Developing efficient and stable catalysts for energy conversion processes such as alkaline oxygen evolution reaction is one of the key measures to solve shortage problems. During evolution, several electrocatalysts would undergo structural reconstruction from pre‐catalyst state real‐catalyst state. The may modify quantity characterizations active sites, thus affecting configuration adsorption strength intermediates, which directly influence activity stability electrocatalysts....

This work provides important insight into the structure–activity relationships of transition metal single-atom catalysts. Various traditional, spectral and electronic descriptors are suggested.

Dual-metal site catalysts (DMSCs) supported on nitrogen-doped graphene have shown great potential in heterogeneous catalysis due to their unique properties and enhanced efficiency. However, the precise control stabilization of metal dimers, particularly oxygen activation reactions, present significant challenges practical applications. In this study, we integrate high-throughput density functional theory calculations with machine learning techniques predict optimize catalytic DMSCs. Transfer...

Electrochemical/thermochemical CO2 reduction reactions (CO2RR) on double-atom catalysts (DACs) have emerged as a novel frontier in energy and environmental catalysis. However, the lack of investigation underlying structure-property relationship greatly limits rational design practical application related catalysts. Herein, we carried out comprehensive theoretical study CO2RR catalyzed by series C2N-supported transition metals to shed light this issue. We demonstrate that activity DAC can be...

Water adsorption and decomposition on stoichiometrically perfect oxygen vacancy containing ZnGa2O4 (100), (110), (111) surfaces were investigated through periodic density functional theory (DFT) calculations. The results demonstrated that water are surface-structure-sensitive processes. On a surface, the most stable molecular could take place involved generation of hydrogen bonds. For dissociative adsorption, energy surface was more than 4 times energies other two surfaces, indicating it to...

The effects of the surface atomic and electronic structures, oxygen defects, hydration on CO2 adsorption ZnGa2O4(100), (110), (111) surfaces were studied using density functional theory (DFT) slab calculations. For perfect (100) surface, most stable state involved Zn-O-Ga bridge site, with an energy 0.16 eV. In case (110) surfaces, strongest binding occurred Zn-O sites, much lower energies -0.22 eV -0.35 eV, respectively. addition, showed activation ability, but dissociation could not...

The performances of nonlinear optics (NLO) and thermally activated delayed fluorescence (TADF) materials are strongly related to the torsion angles (θ) between donor (D) acceptor (A) moieties in D-A architecture molecules. However, underlying relationships connecting θ NLO/TADF remain unclear. Herein, we present a comprehensive theoretical study on composed series backbone molecules (TPAAP/TPAAQ AQ-DMAC/AQ-MeFAC series) shed light these relationships. It is found that changing via...

Pt-based catalyst is widely used in CO oxidation, while its catalytic activity often undermined because of the poisoning effect. Here, using density functional theory, we propose use a Ru-Pt bimetallic cluster supported on TiO2 for to achieve both high and low Excellent obtained Ru1Pt7/TiO2(101) system, which ascribed strong electric fields induced by charge polarization between one Ru atom neighboring Pt atoms. Because lower electronegativity, donates electrons Pt. This induces around...

Using density functional theory (DFT) calculations, we performed a thorough theoretical investigation on the catalytic mechanism of oxidative self-coupling methanol with molecular oxygen Au-Ag catalysts. It is found that can be activated via hydroperoxyl (OOH) intermediate by taking hydrogen atom from co-adsorbed an energy barrier 0.51 eV, which actually rate determining step for overall reaction. The O, OH and OOH oxidant formation proceeds two channels I II low barriers. We demonstrated...

Sharp carbon-tip on defective graphene oxide induces strong local electric field Pt-site, offering high catalytic performance.