Single-atom Catalysts Research Articles

Nature-Inspired N, O Co-Coordinated Manganese Single-Atom Catalyst for Efficient Hydrogen Peroxide Electrosynthesis.

The two-electron oxygen reduction reaction (2e- ORR) is a pivotal pathway for the distributed production of hydrogen peroxide (H2O2). In nature, enzymes containing manganese (Mn) centers can convert reactive oxygen species into H2O2. However, Mn-based heterogeneous catalysts for 2e- ORR are scarcely reported. Herein, we developed a nature-inspired single-atom electrocatalyst comprising N, O co-coordinated Mn sites, utilizing carbon dots as the modulation platform (Mn CD/C). As-synthesized Mn CD/C exhibited exceptional 2e- ORR activity with an onset potential of 0.786 V and a maximum H2O2 selectivity of 95.8 %. Impressively, Mn CD/C continuously produced 0.1 M H2O2 solution at 200 mA/cm2 for 50 h in the flow cell, with negligible loss in activity and H2O2 faradaic efficiency, demonstrating practical application potential. The enhanced activity was attributed to the incorporation of Mn atomic sites into the carbon dots. Theoretical calculations revealed that the N, O co-coordinated structure, combined with abundant oxygen-containing functional groups on the carbon dots, optimized the binding strength of intermediate *OOH at the Mn sites to the apex of the catalytic activity volcano. This work illustrates that carbon dots can serve as a versatile platform for modulating the microenvironment of single-atom catalysts and for the rational design of nature-inspired catalysts.

Single-Atom Pt Loaded on MOF-Derived Porous TiO2 with Maxim-Ized Pt Atom Utilization for Selective Hydrogenation of Halonitro-benzene.

The location control of single atoms relative to supports is challenging for single-atom catalysts, leading to a large proportion of inaccessible single atoms buried under supports. Herein, a "sequential thermal transition" strategy is developed to afford single-atom Pt preferentially dispersed on the outer surface of TiO2. Specifically, a Ti-MOF confining Pt nanoparticles is converted to PtNPs and TiO2 composite coated by carbon (PtNPs&TiO2@C-800) at 800 °C in N2. Subsequent thermal-driven atomization of PtNPs at 600 °C in air produce single-atom Pt decorated TiO2 (Pt1/TiO2-600). The resulting Pt1/TiO2-600 exhibits superior p-chloroaniline (p-CAN) selectivity (99 %) to PtNPs/TiO2-400 (45 %) and much better activity than Pt1@TiO2-600 with randomly dispersed Pt1 both outside and inside TiO2 in the hydrogenation of p-chloronitrobenzene (p-CNB). Mechanism investigations reveal that Pt1/TiO2-600 achieves 100 % accessibility of Pt1 and preferably adsorbs the -NO2 group of p-CNB while weakly adsorbs -Cl group of p-CNB and p-CAN, promoting catalytic activity and selectivity.

Theoretical Study on Pt1/CeO2 Single Atom Catalysts for CO Oxidation

Understanding the influence of structural configurations on catalytic performance is crucial for optimizing atom‐efficient single‐atom catalysts (SACs). In this study, we conducted a density functional theory (DFT) investigation of single Pt atoms positioned at step‐edges and within a solid solution on the CeO2(111) surface. We compared these configurations in terms of thermodynamic stability, electronic properties, and further potential energy surfaces for CO oxidation. Stability studies revealed that the solid solution catalyst exhibits greater stability compared to the step‐edge catalyst. Additionally, the Pt in the solid solution catalyst can effectively activate lattice oxygen atoms, making the catalyst more conducive to the formation of oxygen vacancies. The CO oxidation process was analyzed using the Mars‐van Krevelen mechanism, revealing that the solid solution catalyst possesses a more moderate CO adsorption energy. This, coupled with its lower oxygen vacancy formation energy, leads to reduced energy barriers throughout the CO oxidation cycle. Our findings highlight the strong dependence of catalytic activity on the specific configuration of Pt atoms within the CeO2 matrix, with the solid solution model demonstrating superior catalytic efficiency compared to the step‐edge‐supported Pt catalysts.

Transition Metals Doped into g-C3N4 via N,O Coordination as Efficient Electrocatalysts for the Carbon Dioxide Reduction Reaction.

The electrochemical carbon dioxide reduction reaction (CO2RR) is a potential and efficient method that can directly convert CO2 into high-value-added chemicals under mild conditions. Owing to the exceptionally high activation barriers of CO2, catalysts play a pivotal role in CO2RR. In this study, the transition metal (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) is doped into g-C3N4 with a unique N,O-coordination environment, namely, TM-N1O2/g-C3N4. Herein, the catalytic performance and reaction mechanism for the CO2RR on TM-N1O2/g-C3N4 are systematically investigated by density functional theory methods. Especially, through the calculation of ΔG*H and ΔG*COOH/ΔG*OCHO, the catalysts with preference for the CO2RR over the hydrogen evolution reaction (HER) are selected for further study. Furthermore, Gibbs free energy computation results of each elementary step for the CO2RR on these catalysts indicate that Ti-N1O2/g-C3N4 has significant catalytic activity and selectivity for reducing CO2 to methanol (CH3OH) with the limiting potential (UL) of -0.55 V. Finally, through frontier molecular orbital theory and charge transfer analyses, the introduction of the O atoms illustrates that it is instrumental in regulating the electron distribution of the catalytic active site, thereby improving the catalytic performance. This work provides insight into the design of single-atom catalysts with unique coordination structures for the CO2RR.

Preparation and Catalytic Properties of Gold Single-Atom and Cluster Catalysts Utilizing Nanoparticulate Mg-Al Layered Double Hydroxides.

Au single atoms and clusters were stabilized on Mg-Al layered double hydroxide nanoparticles (LDH NPs), and the obtained Au@LDH NPs were supported on SiO2 and CeO2. After hydrogen reduction, Au single atoms were found together with Au clusters on LDH/SiO2. In contrast to Au single-atom catalysts which are deposited in metal vacancies of oxide supports, the LDH NPs stabilize very small Au species despite the absence of metal vacancies. The obtained Au(0)@LDH/SiO2 catalyzed aerobic oxidation of alcohols, and Au single atoms maintained after the reaction. Given that only Au NPs were observed on bulk LDH, the abundant surface OH group of LDH NPs would contribute to stabilize Au, resulting in higher activity than Au/LDH-bulk. After calcination to transform LDH to mixed metal oxide (MMO), the obtained Au(0)@MMO/SiO2 also exhibited high catalytic activity. Moreover, Au(0)@LDH/CeO2 exhibited higher activity and excellent selectivity for hydrogenation of 4-nitrostyrene to 4-aminostyrene than conventional Au catalysts such as Au/CeO2 and Au/TiO2. We demonstrated that Au size can be minimized using LDH NPs, exhibiting high catalytic performance. The basic surface OH groups of LDH would be also beneficial for deprotonation of alcohols and heterolytic dissociation of H2 in the catalytic reactions.

Demystifying Synergistic Multifunctional Electrocatalysis of N-Doped Graphene/WS2 Heterostructure with Single-Atom Catalysts for Water Splitting and Fuel Cells.

As the demand for sustainable energy continues to rise, electrocatalysis has become increasingly prominent in the advancement of clean energy technologies. By scrutinizing the material to function as a multifunctional catalyst, the effectiveness of energy conversion processes is significantly enhanced. This study focuses on harnessing graphene/WS2 van der Waals heterostructures for overall water splitting and fuel cell applications, using transition metals (TMs) from Sc-Zn as single-atom catalysts (SACs). Additionally, the research explores the synergistic effect of nitrogen doping combined with SACs to modify the material into multifunctional catalysts. The stability of all TMs as SACs in the vdW heterostructure (TM@GW) and nitrogen-doped TM@GW (TM@NGW) is validated with negative cohesive and formation energies, and thermodynamic stability is also corroborated with ab initio molecular dynamics (AIMD) analysis at both 300 and 500 K for 5 ps. The observed electrocatalytic performance of TM@GW and TM@NGW depicts that the Ni@NGW system exhibits trifunctional property with the lowest overpotentials {ηHER; ηOER; ηORR = 0.21; 0.42; 0.27 V}. Additionally, the Cr@NGW material displays bifunctional catalytic activity for the OER and ORR, with overpotentials of 0.53 and 0.37 V, respectively. The synergistic effect between N doping and SACs is further studied with the d, p band centers and density of states calculations. Furthermore, the scaling relation between the adsorption of intermediates and reaction kinetics is studied, which validates the coaction of N and SACs in the TM@NGW heterostructure. This study demonstrates that the inclusion of SACs and nitrogen atoms in the GW heterostructure significantly enhances the catalytic performance by approximately 26%, effectively transforming the system into a multifunctional catalyst. These findings emphasize the role of SACs in vdW heterostructures and N doping effects, providing valuable insights to guide the design of advanced catalysts for water splitting and fuel cell applications.

Two-Dimensional Topological Platinum Telluride Superstructures with Periodic Tellurium Vacancies for Efficient and Robust Catalysis.

Defect engineering in the inherently inert basal planes of transition metal dichalcogenides (TMDs), involving the introduction of chalcogen vacancies, represents a pivotal approach to enhance catalytic activity by exposing high-density catalytic metal single-atom sites. However, achieving a single-atom limit spacing between chalcogen vacancies to form ordered superstructures remains challenging for creating uniformly distributed high-density metal single-atom sites on TMDs comparable to carbon-supported single-atom catalysts (SACs). Here we unveil an efficient TMD-based topological catalyst for hydrogen evolution reaction (HER), featuring high-density single-atom reactive centers on a few-layer (7 × 7)-PtTe2-x superstructure. Compared with pristine Pt(111), PtTe2, and (2 × 2)-PtTe2-x, (7 × 7)-PtTe2-x exhibits superior HER performance owing to its substantially increased density of undercoordinated Pt sites, alongside exceptional catalytic stability when operating at high current densities. First-principles calculations confirm that multiple types of undercoordinated Pt sites on (7 × 7)-PtTe2-x exhibit favorable hydrogen adsorption Gibbs free energies, and remain active upon increasing hydrogen coverage. Furthermore, (7 × 7)-PtTe2-x possesses nontrivial band topologies with robust edge states, suggesting potential enhancements for HER. Our findings are expected to advance TMD-based catalysts and exploration of topological materials in catalysis.

Unveiling the spin adaptability of electrocatalytic nitrogen reduction catalyzed by Fe, Ru and Os-anchored nitrogen-doped graphene

It is of a great challenge to achieve efficient single-atom catalysts (SACs) for electrocatalytic nitrogen reduction. Especially, the SACs from transition metals have complex electron conformation. It is urgently necessary to examine the effect of spin state of transition metals on the catalytic performance of SACs for nitrogen fixed. In this work, using density functional theory (DFT) calculations, we firstly evaluated the catalytic capability of 21 transition metals to achieve the most potential metals with the special electron conformation of d6, including Fe, Ru and Os, to construct SACs. Our examinations revealed that the catalytic performance of SAC for nitrogen reduction increases with the decrease of the spin multiplicity for the same metal through the same reaction pathway and further improves with the increase of period number of transition metal. Additionally, the selectivity of SAC for nitrogen reduction reaction also increases with the increase of period over hydrogen evolution reaction under the low spin state. Finally, we found that the OsN4C catalysts had excellent catalytic performance for nitrogen reduction with the extremely low overpotential (0.03V) through the distal reaction path under the low spin state, which were expected to be the potential industrial applications for electrocatalytic nitrogen reduction.

FeN4S1 Single-Atom Sites Anchored on Three-Dimensional Porous Carbon for Highly Efficient and Durable Oxygen Electrocatalysis.

Precisely designing asymmetric active centers and exploring their electronic regulation effects to prepare efficient bifunctional single-atom catalysts (SACs) is important for boosting the practical applications of zinc-air batteries (ZABs). Herein, an effective strategy has been developed by introducing an axial S atom to the FeN4 active center, simultaneously assisted by pyrolyzing the graphene oxide (GO) sheathed zeolitic-imidazolate framework-8 (ZIF8) composite and constructing a three-dimensional (3D) porous framework with abundant FeN4S1 moieties. This structure can accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics owing to the modulated electronic redistribution and d-band center with a reduced energy barrier. The optimal S-Fe-NC/rGO showcases a lower voltage gap (ΔE) of 0.64 V between both the ORR and OER half-wave potentials at 10 mA cm-2, highlighting the excellent bifunctional activities. The assembled S-Fe-NC/rGO rechargeable liquid ZABs deliver a power density of 154.05 mW·cm-2 and a desirable durability of >900 h. More importantly, the corresponding flexible solid-state ZABs exhibit considerable foldability.

Synergetic Modulation of Electronic Properties of Cobalt Oxide via "Tb" Single Atom for Uphill Urea and Water Electrolysis.

Exploring single-atom (SA) catalysts in hybrid urea-assisted water electrolysis offers a viable alternative to both Hydrogen (H2) generation and polluted water treatment. However, the unfavorable electronic stabilization, low SA content, intrinsically slow kinetics, and imbalanced adsorption-desorption steps are the bottleneck for its scale-up implementation. Herein, a rare-earth Terbium single atom (TbSA) is topologically stabilized on defect-rich Co3O4 (TbSA@d-Co3O4) by Tb─O co-ordination for urea oxidation reaction (UOR) and H2 evolution reaction (HER). Benefitting from the strong TbSA interaction with the d-Co3O4, the TbSA@d-Co3O4 achieves a 10mAcm-2 current density at 1.27V and -35mV for UOR and HER, respectively. Remarkably, when TbSA@d-Co3O4 is applied as a bi-functional catalyst in a two-electrode system, it merely requires 1.22V to acquire 10mAcm-2 with excellent operational stability for 100 h. The hybrid electrolyzer can be successfully empowered by the triboelectric nanogenerator, AA battery, and solar panel with a nominal potential of 1.5V. The mechanistic investigation predicts "TbSA" insertion in d-Co3O4 lowered the potential determining step, attributed to balanced reaction energetics for adsorption-desorption of intermediates and favorable charge transfer characteristics for UOR. This work offers a new paradigm to explore the catalytic properties of rare-earth "f-block" elements to create advanced electrocatalysts via structural modulation.

Fine Engineering of d-Orbital Vacancies of ZnN4 via High-Shell Metal and Nonmetal Single-Atoms for Efficient and Poisoning-Resistant ORR.

Atomically dispersed metal-nitrogen-carbon (M-N-C) materials are active oxygen reduction reaction (ORR) catalysts. Among M-N-C catalysts, ZnN4 single-atom catalysts (SACs) due to a nearly full 3d10 electronic configuration insufficiently activate oxygen and display low ORR activity. To finely engineer d-orbital vacancies of ZnN4, we combine high-shell metal and nonmetal SAs as electronic regulators that are ZnN4Cl and carbon vacancy-hosted -Cl motifs, which show complementary electron-withdrawing capacities versus the ZnN4. Under that, the ZnN4 exhibits significantly enhanced ORR activity with a half-wave potential (E1/2) of 0.912 VRHE relative to the unmodified ZnN4 (E1/2 = 0.822 VRHE) and simultaneously robust durability (negligible activity loss after 10,000 potential cycles). Particularly, the engineered ZnN4 possesses high resistance to SCN- poisoning, which is rarely achieved among M-N-C SACs. Our works show that combining high-shell metal and nonmetal SAs can finely engineer d-orbital vacancies of metal centers to an optimal state, thereby intrinsically enhancing their catalytic performance.

Location-Specific Microenvironment Modulation Around Single-Atom Metal Sites in Metal-Organic Frameworks for Boosting Catalysis.

Despite coordination environment of catalytic metal sites has been recognized to be of great importance in single-atom catalysts (SACs), a significant challenge remains in the understanding how the location-specific microenvironment in the higher coordination sphere influences their catalysis. Herein, a series of Cu-based SACs, namely Cu1/UiO-66-X (X = -NO2, -H, and -NH2), are successfully constructed by anchoring single Cu atoms onto the Zr-oxo clusters of metal-organic frameworks (MOFs), i.e. UiO-66-X. The -X functional groups dangling on the MOF linkers could be regarded as location-specific remote microenvironment to regulate electronic properties of the single Cu atoms. Remarkably, they exhibit significant differences in the catalysis toward the hydroboration of alkynes. The activity follows the order of Cu1/UiO-66-NO2 ˃ Cu1/UiO-66 ˃ Cu1/UiO-66-NH2 under identical reaction conditions, where Cu1/UiO-66-NO2 showcases the phenylacetylene conversion of 92%, ~3.5 times higher efficiency than that of Cu1/UiO-66-NH2. Experimental and calculation results jointly support that the Cu electronic structure is modulated by the location-specific microenvironment, thereby regulating the product desorption and promoting the catalysis.

Consolidating the Oxygen Reduction with Sub-Polarized Graphitic Fe-N4 Atomic Sites for an Efficient Flexible Zinc-Air Battery.

The effectuation of the Zn-air battery (ZAB) is appealing for active and durable catalysts to kinetically drive the sluggish cathodic oxygen reduction reaction (ORR). Atomic metal-Nx-C sites are widely witnessed with Pt-like activity, but their demetalations still severely restrict the durability in ORR. Here we have profiled an ordered hierarchical porous carbon supported Fe-N4 single-atom (FeNC) catalyst by a template derivation method for efficient ORR and flexible ZAB studies. The FeNC structure is observed with a sub-polarized graphitic Fe-N4 coordination with a shortened Fe-N bond for potentially consolidating the ORR, together with the hierarchical porous matrix for kinetical mass transfer. Resultantly, the optimized FeNC catalyst showcases Pt-beyond alkaline ORR activity (E1/2 = 0.95 V) with long-term durability for 100 h, delivering the flexible ZAB device with high power density (251 mW cm-2) and durable cycle life (80 h). This research underscores the criterion in rationalizing active and robust ORR catalysts through metal-nitrogen bond modulation.

Reductive Coupling of N-Heteroarenes and 1,2-Dicarbonyls for Direct Access to γ-Amino Acids, Esters, and Ketones Using a Heterogeneous Single-Atom Iridium Catalyst.

Despite their significant importance, the challenges in direct and diverse synthesis of N-heterocyclic γ-amino acids/esters/ketones hamper exploration of their applications. Herein, by developing a multifunctional heterogeneous iridium single-atom catalyst composed of silica-confined iridium species and a boron-doped ZrO2 support (Ir-SAs@B-ZrO2/SiO2), we describe its utility in establishing a new reductive coupling reaction of N-heteroarenes and 1,2-dicarbonyls for selective and diverse construction of the as-described compounds in a straightforward manner. The striking features, including good substrate and functionality tolerance, high step and atom economy, exceptional catalyst reusability, and diversified product post-transformations, highlight the practicality of the developed chemistry. Mechanistic studies reveal that the synergy between the active Ir sites and acidic support favors a chemoselective reduction of the more inert N-heteroarenes and affords requisite enamine intermediates. In this work, the concept on precise transformation of reductive intermediates will open a door to further develop useful tandem reactions by rational catalyst design.

Prediction of holey graphyne-supported single atom catalyst for nitrogen reduction reaction by interpretable machine learning and first-principles calculations

The electrocatalytic nitrogen reduction reaction (NRR) with efficient and selective electrocatalysts has emerged as a promising alternative for sustainable ammonia synthesis. In this study, we designed a novel class of single-atom catalysts (SACs), denoted as TM@HGY, by embedding 3d, 4d, and 5d transition metals into synthesized holey graphyne (HGY), and investigated their potential for NRR using a combined approach of density functional theory (DFT) calculations and machine learning. Through stability assessments and a three-step screening strategy, Sc@HGY, V@HGY, and Mo@HGY were identified as promising NRR electrocatalysts. Notably, V@HGY exhibited an exceptionally low limiting potential of −0.16 V, which is superior to all the known NRR SACs supported by graphyne-family members. Machine learning (ML) analysis revealed that the Mendeleev number (Nm), group (G), and d-orbital radius (Rd) of the absorbed metal atom are the primary contributors to the structural stability and catalytic activity of these SACs, and clear strategies for optimizing catalyst design were further suggested based on their intrinsic relationships. This work reveals the significant potential of TM@HGY in NRR, providing powerful guidance for designing high-performance SACs in the field of sustainable ammonia synthesis.

Surface Coordination Chemistry of Graphitic Carbon Nitride from Ag Molecular Probes.

Graphitic carbon nitride (g-C3N4) has gained significant attention for its catalytic properties,especiallyin the development of Single Atom Catalysts (SACs).However,the surface chemistry underlying the formation of these isolated metal sites remains poorly understood.In thisstudyweemploy Surface OrganoMetallic Chemistry (SOMC) together with advanced microscopic and spectroscopic techniquesfor an in-depth analysis of functionalizedg-C3N4materials, where tailored organosilver probe molecules are used to monitor surface processes and characterize resulting surface species. Amulti-technique approach-including high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM), X-ray absorption spectroscopy (XAS), and multinuclear solid-state Nuclear Magnetic Resonance spectroscopy (ssNMR),coupled with density functional theory (DFT) calculations- identifies three primary surface speciesin Ag-functionalized g-C3N4:bis-NHC-Ag+, dispersed Ag+sites, andphysisorbed molecular precursor.These findings highlight a dynamic grafting process and provide insights into the surface coordination chemistryof functionalizedg-C3N4materials.

Electrocatalysts for the Formation of Hydrogen Peroxide by Oxygen Reduction Reaction.

Hydrogen peroxide (H2O2) is a widely used strong oxidant, and its traditional preparation methods, anthraquinone method, and direct synthesis method, have many drawbacks. The method of producing H2O2 by two-electron oxygen reduction reaction (2e- ORR) is considered an alternative strategy for the traditional anthraquinone method due to its high efficiency, energy saving, and environmental friendliness, but it remains a big challenge. In this review, we have described the mechanism of ORR and the principle of electrocatalytic performance testing, and have summarized the standard performance evaluation techniques for electrocatalysts to produce H2O2. Secondly, according to the theoretical calculation and experimental results, several kinds of efficient electrocatalysts are introduced. It is concluded that noble metal-based materials, carbon-based materials, non-noble metal composites, and single-atom catalysts are the preferred catalyst materials for the preparation of H2O2 by 2e- ORR. Finally, the advantages and novelty of 2e- ORR compared with traditional methods for H2O2 production, as well as the advantages and disadvantages of the above-mentioned high-efficiency catalysts, are summarized. The application prospect and development direction of high-efficiency catalysts for H2O2 production by 2e- ORR has been prospected, which is of great significance for promoting the electrochemical yield of H2O2 and developing green chemical production.

Engineering Metal‐Support Interaction for Manipulate Microenvironment: Single‐Atom Platinum Decorated on Nickel‐Chromium Oxides Toward High‐Performance Alkaline Hydrogen Evolution

AbstractRational construction of platinum (Pt)‐based single‐atom catalysts (SACs) with high utilization of active sites holds promise to achieve superior electrocatalytic alkaline HER performance, which requires the assistance of functional supports. In this work, a novel catalytic configuration is reported, namely, Pt SACs anchored on the nickel‐chromium oxides labeled as Pt SACs‐NiCrO3/NF. The mechanism associated with the metal‐support interaction (MSI) for synergy co‐catalysis that empowers efficient HER on Pt SACs‐NiCrO3/NF is clarified. Specifically, the modulated electron structure in Pt SACs‐NiCrO3 manipulates the interface microenvironment, mediating a more free water state, which is beneficial to accelerate front water dissociation behavior on the oxide support. Besides, the homogeneously distributed Pt sites with the created near‐acidic state ensure the subsequent fast proton‐involved reaction. All these determine the comprehensively accelerating HER kinetics. Consequently, Pt SACs‐NiCrO3/NF deliverers considerable HER performance, with overpotentials (η10/η100) of 23/122 mV, high mass activity of 382.77 mA mg−1Pt. When serving in an alkaline water‐based anion exchange membrane electrolytic cell (AEMWE), Pt SACs‐NiCrO3/NF also presents excellent performance (100 mA cm−2 at the cell voltage of 1.51 V and stable up to 100 h), confirming its good prospect.

Polyoxometalates‐Mediated Selectivity in Pt Single‐Atoms on Ceria for Environmental Catalysis

AbstractOptimizing the reactivity and selectivity of single‐atom catalysts (SACs) remains a crucial yet challenging issue in heterogeneous catalysis. This study demonstrates selective catalysis facilitated by a polyoxometalates‐mediated electronic interaction (PMEI) in a Pt single‐atom catalyst supported on CeO2 modified with Keggin‐type phosphotungstate acid (HPW), labeled as Pt1/CeO2‐HPW. The PMEI effect originates from the unique arrangement of isolated Pt atoms and HPW clusters on the CeO2 support. Electrons are transferred from the ceria support to the electrophilic tungsten in HPW clusters, and subsequently, Pt atoms donate electrons to the now electron‐deficient ceria. This phenomenon enhances the positive charge of Pt atoms, moderating O2 activation and limiting lattice oxygen mobility compared to the conventional Pt1/CeO2 catalyst. The resulting electronic structure of Pt combined with the strong and local acidic environment of HPW on Pt1/CeO2‐HPW leads to improved efficiency and N2 selectivity in the degradation of NH3 and NO, as well as increased CO2 yield when inputting volatile organic compounds. This study sheds the light on the design of SACs with balanced reactivity and selectivity for environmental catalysis.

Investigation of Single Atom Catalysts by X‐Ray Absorption Spectroscopy

Investigation of Single Atom Catalysts by X‐Ray Absorption Spectroscopy