Single Pd Research Articles

Catalytic Synergy between Pd Nanoclusters and Ligand-Functionalized Layered Silicates for Improved Formic Acid Dehydrogenation.

The synthesis and stabilization of Pd nanoclusters on a support, as well as simultaneously achieving optimal catalytic activity, remain challenging tasks. Functionalizing the support surface with specific ligands offers a promising solution, but it often requires carefully balancing trade-offs between the reaction yield and catalyst stability. Here, we used two different ligands (propylamine and propylthiol) to functionalize the layered silicate's interlayer surface for Pd nanocluster synthesis and stabilization. For dehydrogenating formic acid, Pd nanoclusters on aminopropyl groups achieved a catalytic activity ∼27-fold higher than that of thiopropyl groups at 70 °C. Our density functional calculations compared the adsorption energetics and bonding characteristics of single Pd atoms and Pd13 nanoclusters on amino- and thio-functionalized silicate surfaces. Pd-N bonds were predicted to be weaker with minimal covalency, while Pd-S bonds exhibit greater covalency due to higher 4d-3p hybridization, resulting in better stability. However, Pd13 clusters undergo severe structural deformation on thiol-functionalized surfaces, resulting in a smaller overall surface area and diminished catalytic stability.

Embedding Single Pd Atoms on NiGa Intermetallic Surfaces for Efficient and Selective Alkyne Hydrogenation.

Catalytic removal of alkynes is essential in industry for producing polymer-grade alkenes from steam cracking processes. Non-noble Ni-based catalysts hold promise as effective alternatives to industrial Pd-based catalysts but suffer from low activity. Here we report embedding of single-atom Pd onto the NiGa intermetallic surface with replacing Ga atoms via a well-defined synthesis strategy to design Pd1-NiGa catalyst for alkyne semi-hydrogenation. The fabricated Pd1Ni2Ga1 ensemble sites deliver remarkably higher specific mass activity under superb alkene selectivity of >96 % than the state-of-the-art catalysts under industry-relevant conditions. Integrated experimental and computational studies reveal that the single-atom Pd synergizes with the neighbouring Ni sites to facilitate the σ-adsorption of alkyne and dissociation of hydrogen while suppress the alkene adsorption. Such synergistic effects confer the single-atom Pd on the NiGa intermetallic with a Midas touch for alkyne semi-hydrogenation, providing an effective strategy for stimulating low active Ni-based catalysts for other selective hydrogenations in industry.

Atomically Dispersed Palladium Catalyst for Chemoselective Hydrogenation of Quinolines.

Chemoselective hydrogenation of quinoline and its derivatives is a significant strategy to achieve the corresponding 1,2,3,4-tetrahydroquinolines (py-THQ) for various potential applications. Here, we precisely constructed a titanium carbide supported atomically dispersed Pd catalyst (PdSA+NC/TiC) for quinoline hydrogenation, delivering above 99% py-THQ selectivity at complete conversion with an outstanding turnover frequency (TOF) of 463 h-1. AC-HAADF-STEM and XAFS demonstrate that the atomic dispersion of Pd includes Pd-Ti2C2 single atoms and Pd clusters with atomic-layer thickness. Theoretical calculation and experimental results revealed that H2 dissociation and subsequent hydrogenation rates were greatly promoted over Pd clusters. Although the adsorption of quinolines and intermediates are easier on Pd clusters than on Pd single atoms, the desorption of py-THQ is more favored over Pd single atoms than over Pd clusters. The desorption step may be the main reason for 5,6,7,8-tetrahydroquinoline (bz-THQ) and decahydroquinoline (DHQ) formation. Thus, a low reaction activity and py-THQ selectivity were received over PdSA/TiC and PdNP/TiC, respectively.

First-principles design of PtPd bimetal dispersed WTe2 monolayer for sensing thermal runaway gases: Enhanced performance against single Pt or Pd dispersion

To conduct the early-monitoring of thermal runaway for the Li-ion battery (LIBs), this work purposes PtPd bimetal dispersed WTe2 (PtPd-WTe2) monolayer as a promising sensing material to realize the high-sensitive detection of thermal runaway gases (H2, CO, CO2, C2H2 and C2H4). The adsorption behavior of PtPd-WTe2 monolayer upon such five gas molecules are compared with single Pt- and Pd-dispersed WTe2 monolayer from the first-principles insight to highlight the combined catalytic property of two noble metal atoms. Results reveal that Pt-, Pd- and PtPd-WTe2 monolayer all behave good chemical and thermal stability at 498 K with good binding force between the noble metal atom(s) and the pristine WTe2 surface. Besides, PtPd-WTe2 monolayer behaves much enhanced adsorption performance with more negative adsorption energy and much higher sensing response with larger bandgap changing rate than Pt- and Pd-WTe2 monolayer upon five typical gas molecules. Moreover, the desorption property analysis manifests the necessity conducting the heating process to realize the reusability of PtPd-WTe2 monolayer for gas sensing. These findings manifest the strong potential of PtPd-WTe2 monolayer as a resistive gas sensor for detections of the thermal runaway gas species thus evaluating the operation status of the LIBs, which may stimulate the further deeper investigations about WTe2-based materials for gas sensing applications across multiple fields.

Revealing the Origin of Graphene Anchored Single Palladium Atom for Electrochemical CO2 Reduction to Syngas with Tunable CO/H2 Ratios

AbstractPd based catalysts are rare metal‐based catalyst to yield tunable CO/H2 ratios for Fischer‐Tropsch synthesis. How to achieve the co‐production of CO and H2 with as little Pd as possible is extremely meaningful for Cn industry. Recent experiment revealed single Pd atom anchored on graphene exhibits high activity for CO2 electroreduction to syngas, yet the origin of activity and controllable CO/H2 ratios, especially the exact Pd coordination structure, remains elusive. Here we employ grand‐canonical density functional theory to show that Pd−N1, rather than the commonly accepted Pd‐N4, serves as the active center, and the charge‐carrying capability is an effective descriptor. The site with more Pd−C coordination can better submerge in graphene‘s delocalized π electrons for higher charge‐carrying capacity to carry excess charges that occupy Pd 4dz2 orbital and promote electron injection. Importantly, the tunable CO/H2 ratio can be explained with difference in charge‐carrying capability of transition state for *COOH and *H2 formation. This work solves the puzzle of coordinating structure of Pd active site and demonstrates the important role of charge‐carrying capability in electrochemical process, which shall provide a reference for further exploration of efficient electrocatalysts.

Study of size effect of palladium atoms as single-atom and clusters nanoparticle catalysts for Heck reactions

We reported a series of nitrogen-doped carbon-supported palladium (Pd) species with various sizes for the Heck reaction of iodobenzene and methyl acrylate. By precisely controlling the synthesis procedure, we have successfully synthesized a range of Pd-based catalysts, including single Pd atom, sub-nanometer Pd clusters (∼ 0.4 nm, and ∼1.6 nm), and Pd nanoparticles (∼5.8 nm and 10 nm). Remarkably, these catalysts exhibit a distinct size-dependent catalytic activity in the Heck reaction. In the case of the Heck reaction of 4‑methoxy-iodobenzene and methyl acrylate, the Pd-10 site demonstrated the highest site-specific turnover frequency (TOF), reaching 792.5 h−1. This performance is impressively 5.2 and 15.6 times superior to that of the Pd1 site (152 h-1) and Pd-10 site (50.6 h-1), respectively. Significantly better in the Heck reactions with other aryl halides were achieved with Pd-1.6/N-C (comprising of approximately 1.6 nm-sized Pd clusters), compared to those containing 10 nm-sized nanoparticles (Pd-10/N-C) or Pd1/N-C. These findings suggested that Pd clusters of around 1.6 nm may serve as the potential catalytic sites for the Heck reaction.

The importance of Pd carbide formation for reactions with ethene and other organic molecules

The reactions of a range of unsaturated hydrocarbons and oxygenated organic molecules with pure Pd surfaces can result in the carbidisation of the bulk of the metal, even though Pd is not usually recognised as a carbide-forming material. This can have important implications for catalysis by Pd. In this personal review it is shown that for the case of ethene, such bulk carbidisation is very fast above about 400 K. Adsorption and reaction with both pure single crystal Pd and supported nanoparticulate Pd is reported. For the former every ethene molecule has a 70 % probability per collision with the surface of dehydrogenating and depositing C into the metal. At low temperature (400 K) this accumulates near the surface, while at higher temperatures the C dissolves in the bulk and is reduced in the surface region. It can be retrieved by treatment in oxygen. For the nanoparticulate metal, the bulk is saturated very quickly with C, ultimately making a Pd4C-like material. During this time a disproportionation reaction occurs in which methane only evolves into the gas phase and C is deposited in the Pd. Once the bulk is saturated with C, then reaction with ethene stops. It is shown that similar carbidisation also takes place with acetaldehyde.

Stabilizing and Activating Active Sites: 1T-MoS2 Supported Pd Single Atoms for Efficient Hydrogen Evolution Reaction.

Metallic 1T-MoS2 with high intrinsic electronic conductivity performs Pt-like catalytic activity for hydrogen evolution reaction (HER). However, obtaining pure 1T-MoS2 is challenging due to its high formation energy and metastable properties. Herein, an in situ SO4 2--anchoring strategy is reported to synthesize a thin layer of 1T-MoS2 loaded on commercial carbon. Single Pd atoms, constituting a substantial loading of 7.2wt%, are then immobilized on the 1T-phase MoS2 via Pd─S bonds to modulate the electronic structure and ensure a stable active phase. The resulting Pd1/1T-MoS2/C catalyst exhibits superior HER performance, featuring a low overpotential of 53mV at the current density of 10mAcm-2, a small Tafel slope of 37mVdec-1, and minimal charge transfer resistance in alkaline electrolyte. Moreover, the catalyst also demonstrates efficacy in acid and neutral electrolytes. Atomic structural characterization and theoretical calculations reveal that the high activity of Pd1/1T-MoS2/C is attributed to the near-zero hydrogen adsorption energy of the activated sulfur sites on the two adjacent shells of atomic Pd.

Hydrodynamics-Controlled Single-Particle Electrocatalysis.

Electrocatalysis is considered promising in renewable energy conversion and storage, yet numerous efforts rely on catalyst design to advance catalytic activity. Herein, a hydrodynamic single-particle electrocatalysis methodology is developed by integrating collision electrochemistry and microfluidics to improve the activity of an electrocatalysis system. As a proof-of-concept, hydrogen evolution reaction (HER) is electrocatalyzed by individual palladium nanoparticles (Pd NPs), with the development of microchannel-based ultramicroelectrodes. The controlled laminar flow enables the precise delivery of Pd NPs to the electrode-electrolyte interface one by one. Compared to the diffusion condition, hydrodynamic collision improves the number of active sites on a given electrode by 2 orders of magnitude. Furthermore, forced convection enables the enhancement of proton mass transport, thereby increasing the electrocatalytic activity of each single Pd NP. It turns out that the improvement in mass transport increases the reaction rate of HER at individual Pd NPs, thus a phase transition without requiring a high overpotential. This study provides new avenues for enhancing electrocatalytic activity by altering operating conditions, beyond material design limitations.

Pd and Pd-B modified g-CN monolayer as innovative sensor and scavenger for CO, NO2, C2H2 and C2H4: A DFT study

The prompt detection of toxic gases like CO, NO2, C2H2, and C2H4 is crucial for both environmental preservation and industrial safety. In this work, we investigate the adsorption behavior and sensing performance of these four gases on both intrinsic g-CN and g-CN modified with single Pd atom and Pd-B pair, denoted as Pd-g-CN and Pd-B-g-CN, respectively, utilizing the first-principles calculations. The results indicate that the introduction of Pd atom and Pd-B pair significantly enhances the adsorption effect of g-CN monolayer toward these gases, with adsorption energies ranging from − 0.44 eV to − 1.43 eV. Furthermore, all adsorptions are identified as chemisorption, with the adsorption strength following the order of NO2 > CO > C2H4 > C2H2. Additionally, the adsorption of NO2, C2H2, and C2H4 induces notable changes in the work function of Pd-g-CN and Pd-B-g-CN, as well as approximately a 20-time increase in the bandgap of Pd-g-CN. Moreover, the Pd-g-CN and Pd-B-g-CN monolayers exhibit reasonable recovery times for C2H2 and C2H4, measured as 0.04 s and 6.40 μs at 298 K, respectively. Furthermore, NO2 can be rapidly desorbed from the Pd-B-g-CN surface at 398 K, with a short recovery time of 8.17 s. Therefore, the Pd-g-CN and Pd-B-g-CN monolayers can be regarded as potential gas-sensitive materials for the detection of C2H2 and C2H4 at room temperature, respectively. These research findings provide robust theoretical support for the design of novel gas sensors and efficient toxic gas adsorbents.

Single atom Pd anchored-MnO confined in porous carbon matrix for low-level VOCs removal at room temperature

Sustainably removing low-level VOCs at room temperature especially in the presence of water vapor has great demand. Herein, single-atom Pd anchored MnO nanoparticles (Pd/MnO) were confined in the hydrophobic porous carbon matrix. As-synthesized Pd/MnO@C exhibited superior removal capacity for VOCs such as hexanal, pentanal and toluene. Under the WHSV of 450 L/g·h, the 99% removal capacity for 15 ppm hexanal at 30 °C and relative humidity (RH) 50% reached 388.8 mg/g, which was 2.4 times as that of commercial BPL activated carbon. In addition, it exhibited much better regeneration ability at low temperature (105 °C) than activated carbon. In-situ DRIFTS and EPR indicated that water vapor mediated the activation of oxygen to form hydroxyl radicals to decompose VOCs. This paper opens a new way to sustainably remove low-level VOCs at room temperature under humid conditions via the hydrophobic carbon confinement effect and single-atom catalysis.

Boosting photocatalytic overall water splitting performance by dual-metallic single Ni and Pd atoms decoration of MoS2: A DFT study

Herein, we propose a novel MoS2 supported single Ni and Pb atoms catalyst (Ni/Pd@MoS2), on which the enhanced efficiency of water splitting is confirmed by quantitative density functional theory (DFT) calculations. The Bader charge, electron density difference (EDD) and projected density of state (PDOS) analysis demonstrates that the moderate electron transfer is reached by the synergy of the Ni atom and the Pd atom. As extra channel for excited carrier migration, the present of defect states obviously prolongs the carrier lifetime (143.45 ps). The unique electronic environment contributes to the electronic synergy and spatially separated of the effective active sites, leading the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) happen smoothly on the Pd and S site, respectively. Our research presents a novel idea for the development of highly efficient diatomic catalysts towards overall water splitting.

Abstract 5769: Target identification of T-cell activating immunomodulatory tetrahydrothiazepines: DGKα and DGKζ inhibitors

Abstract We became interested in bicyclic tetrahydrothiazepine derivatives described in a Patent (WO 2016/139181) having immunomodulatory activities on CD3-activated T cells (CD4+ & CD8+) and NK cell increasing the secretion of several cytokines such as, e.g., IL-2, IFN-γ and/or TNF-α whereas corresponding unstimulated immune cells do not respond. Surprisingly - in contrast to what has been described in the patent - the N-H of the Amides 1 and 2 described in the patent was not required for potency and the oxadiazoles 1 and 2 were significantly more potent in T-cell proliferation and IL-2 release. Compound 1 was in vivo active in a single dose PD study in mice after CD3 activation and in a MC38 xenograft mice model showing single agent activity. Amide 1 and Amide 2 were identified in a phenotypic screen and the mode of action was unknown. Because of the promising pharmacological profile and in vivo activity, we were interested in the target. Here we describe how we identified the potential targets DGKα and DGKζ. Citation Format: Thomas Luebbers, Adrian Britschgi, Veronica Costa, Thomas Friess, Jean-Christophe Hau, Gordon Heidkamp, Holger Kuehne, Laetitia J. Martin, Filip Roudnicky, Manuel Tzouros, An Vandemeulebroucke. Target identification of T-cell activating immunomodulatory tetrahydrothiazepines: DGKα and DGKζ inhibitors [abstract]. In: Proceedings of the American Association for Cancer Research Annual Meeting 2024; Part 1 (Regular Abstracts); 2024 Apr 5-10; San Diego, CA. Philadelphia (PA): AACR; Cancer Res 2024;84(6_Suppl):Abstract nr 5769.

Abstract 1129: A multifaceted study of X-Ray radiation therapy across diverse mouse tumor models

Abstract In this study, we showcase the application of X-ray radiation therapy of tumor-bearing mice across 13 syngeneic tumors, one intracranial tumor, and in combination with radiosensitizing drugs, aiming to develop potent cancer treatment strategies. 1.We examined the effects of different radiation levels on multiple tumor models using a therapeutic device delivering targeted radiation to the tumor site. 2.We investigated the combined benefits of radiation with the radiosensitizer Gemcitabine on the H22 liver tumor model. 3.We assessed the impact of radiation sensitization on the HCC1975-luc intracranial tumor model in combination with AZD0156, a drug that cannot cross the blood-brain barrier. The integrity of the blood-brain barrier and the presence of the pharmacodynamic marker pRAD50 of AZD0156 were evaluated. The results show that X-ray radiation has anti-tumor effects across diverse models, with combination drug treatment with both Gemcitabine and AZD0156 showing enhanced therapeutic effects. Furthermore, pRAD50 showed decreasing trend in the single dose PD study in HCC1975-luc intracranial model. We conclude that our platform provides robust methods for evaluating the therapeutic effects of X-Ray radiation, offering invaluable insights for the creation of new cancer therapies. Citation Format: Jingqi Huang, Wentao Li, Xiaoyan He, Weiwei Cheng, Lingyun Zhang, Guannan Li, Qiuliang Li, Yongfei Wang, Xuesong Ren, Zhi Wei, Long Shi, Yiran Wei, Jing Jin, Linfeng Li, Wei Yun. A multifaceted study of X-Ray radiation therapy across diverse mouse tumor models [abstract]. In: Proceedings of the American Association for Cancer Research Annual Meeting 2024; Part 1 (Regular Abstracts); 2024 Apr 5-10; San Diego, CA. Philadelphia (PA): AACR; Cancer Res 2024;84(6_Suppl):Abstract nr 1129.

Atom-Pd catalysts supported by hollow N-doped carbon nanospheres for ultra-efficient nitrogen reduction reaction

Electrochemical N2 reduction reaction (eNRR) presents a promising alternative to the Haber-Bosch process, owing to its mild preparation conditions, absence of costly reagents, and high energy conversion efficiency. However, the process poses significant challenges due to its poor selectivity and low yield. Here, single atom Pd is successfully anchored on N-doped hollow carbon nanospheres via a simple wet impregnation method under relatively mild loading temperature, anhydrous and anaerobic environments. Our experiment demonstrates that SA-Pd/N@C exhibits outstanding catalytic performance in comparison to Pd nanoparticles which is consistent with the results of the DFT calculations, achieving an NH3 yield rate of 132.8 μg·h − 1·mgcat−1 and a corresponding FE of 6 % at -0.2 V versus RHE in HCl electrolyte (pH=1), as well as superior stability with only 5 % decrease after 10 consecutive cycles of electrochemical testing at room temperature, positioning it as one of the most effective catalyst materials reported for eNRR. The exceptional eNRR activity and stability can be attributed to the abundant active sites resulting from the relatively mild loading temperature, as well as electronic effects and structural engineering, which further diminish *H adsorption and efficiently suppress hydrogen evolution reaction. This work will provide a novel approach to enhance the eNRR performance through the effective design of Pd single-atom catalyst

Ab initio morphology prediction of Pd, Ag, Au, and Pt nanoparticles on (0001) sapphire substrates

We energetically predict the morphology of Pd, Ag, Au, and Pt nanoparticles on (0001) sapphire substrates, using density functional theory (DFT) simulations and the well-known Young–Dupre equation. In all cases, the contact angles exceed 90°, indicating that the nanoparticles are spherical. Notably, Au nanoparticles exhibit a higher contact angle than those of their counterparts. The validity of the proposed abinitio nanoparticle morphology prediction approach based on DFT simulations was assessed in comparison with our previous experimental findings pertaining to the time variation of the full width at half maximum (FWHM) of the resonant peak. Furthermore, the diffusivities of single Pd, Ag, Au, and Pt atoms on the substrate were evaluated by calculating the activation energy, offering insights into the underlying physics governing the timing of FWHM peaks. The analysis confirms a higher diffusivity of Au and Ag compared with Pd and Pt. According to the comparison between DFT and experiment results, although no clear relation is observed between the contact angles and timing of FWHM peaks, the diffusivity of sputtered atoms may influence the timing of FWHM peaks. Thus, timing can help to clarify the nanoparticle size, rather than shape.

Position Tracking Control of 4-DOF Underwater Robot Leg Using Deep Learning

This paper presents a novel hybrid control method for position tracking of an underwater quadruped walking robot. The proposed approach combines an existing position-tracking control method with a deep-learning neural network. The neural network compensates for non-linear dynamic characteristics, such as the effect of fluid, without relying on mathematical modeling. To achieve this, a Multi-Layer Perceptron neural network is designed to analyze joint torque in relation to the joint angle and angular velocity of the robot, as well as the position and orientation of the foot tip and environmental data. The improvement in tracking control performance is evaluated using a 4-DOF underwater robot leg. For the neural network design, position tracking control data, including dynamic characteristics, were collected through position command-based position tracking control. Afterward, a learning model was constructed and trained to predict joint torque related to the robot’s motion and posture. This learning process incorporates non-linear dynamic characteristics, such as joint friction and the influence of fluid, in the joint torque prediction. The proposed method is then combined with conventional task-space PD control to perform position-tracking control with enhanced performance. Finally, the proposed method is evaluated using the underwater robot leg and compared to a single task-space PD controller. The proposed method demonstrates higher position accuracy with similar joint torque output, thereby increasing compliance and tracking performance simultaneously.

Feeble Single-Atom Pd Catalysts for H2 Production from Formic Acid.

Single-atom catalysts are thought to be the pinnacle of catalysis. However, for many reactions, their suitability has yet to be unequivocally proven. Here, we demonstrate why single Pd atoms (PdSA) are not catalytically ideal for generating H2 from formic acid as a H2 carrier. We loaded PdSA on three silica substrates, mesoporous silicas functionalized with thiol, amine, and dithiocarbamate functional groups. The Pd catalytic activity on amino-functionalized silica (SiO2-NH2/PdSA) was far higher than that of the thiol-based catalysts (SiO2-S-PdSA and SiO2-NHCS2-PdSA), while the single-atom stability of SiO2-NH2/PdSA against aggregation after the first catalytic cycle was the weakest. In this case, Pd aggregation boosted the reaction yield. Our experiments and calculations demonstrate that PdSA in SiO2-NH2/PdSA loosely binds with amine groups. This leads to a limited charge transfer from Pd to the amine groups and causes high aggregability and catalytic activity. According to the density functional calculations, the loose binding between Pd and N causes most of Pd's 4d electrons in amino-functionalized SiO2 to remain close to the Fermi level and labile for catalysis. However, PdSA chemically binds to the thiol group, resulting in strong hybridization between Pd and S, pulling Pd's 4d states deeper into the conduction band and away from the Fermi level. Consequently, fewer 4d electrons were available for catalysis.

Electron-enriched single-Pd-sites on g-C3N4 nanosheets achieved by in-situ anchoring twinned Pd nanoparticles for efficient CO2 photoreduction

Modulating electronic structures of single-atom metal cocatalysts is vital for highly active photoreduction of CO2, and it's especially challenging to develop a facile method to modify the dispersion of atomical photocatalytic sites. We herein report an ion-loading pyrolysis route to in-situ anchor Pd single atoms as well as twinned Pd nanoparticles on ultra-thin graphitic carbon nitride nanosheets (PdTP/PdSA-CN) for high-efficiency photoreduction of CO2. The anchored Pd twinned nanoparticles donate electrons to adjacent single Pd–N4 sites through the carbon nitride networks, and the optimized PdTP/PdSA-CN photocatalyst exhibits a CO evolution rate up to 46.5 ​μmol ​g−1 ​h−1 with nearly 100% selectivity. As revealed by spectroscopic and theoretical analyses, the superior photocatalytic activity is attributed to the lowered desorption barrier of carbonyl species at electron-enriched Pd single atoms, together with the improved efficiencies of light-harvesting and charge separation/transport. This work has demonstrated the engineering of the electron density of single active sites with twinned metal nanoparticles assisted by strong electronic interaction with the support of the atomic metal, and unveiled the underlying mechanism for expedited photocatalytic efficiency.

Theoretical insights into single-atom catalysts for improved charging and discharging kinetics of Na-S and Na-Se batteries.

Dissolution of poly-sulfide/selenides (p-S/Ses) intermediates into electrolytes, commonly known as the shuttle effect, has posed a significant challenge in the development of more efficient and reliable Na-S/Se batteries. Single-atom catalysts (SACs) play a crucial role in mitigating the shuttling of Na-pS/Ses and in promoting Na2S/Se redox processes at the cathode. In this work, single transition metal atoms Co, Fe, Ir, Ni, Pd, Pt, and Rh supported in nitrogen-deficient graphitic carbon nitride (rg-C3N4) are investigated to explore the charging and discharging kinetics of Na-S and Na-Se batteries using Density Functional Theory calculations. We find that SAs adsorbed on reduced g-C3N4 monolayers are substantially more effective in trapping higher-order Na2Xn than pristine g-C3N4 surfaces. Moreover, our ab initio molecular dynamics calculations indicate that the structure of X8 (X = S, Se) remains almost intact when adsorbed on Fe, Co, Ir, Ni, Pt, and Rh SACs, suggesting that there is no significant S or Se poisoning in these cases. Additionally, SACs reduce the free energies of the rate-determining step during discharge and present a lower decomposition barrier of Na2X during charging of Na-X electrode. The underlying mechanisms behind this fast kinetics are thoroughly examined using charge transfer, bonding strength, and d-band center analysis. Our work demonstrates an effective strategy for designing single-atom catalysts and offers solutions to the performance constraints caused by the shuttle effect in sodium-sulfur and sodium-selenium batteries.