Ag-based Catalysts Research Articles

Evaluating electrocatalytic activities of Pt, Pd, Au and Ag-based catalyst on PEMFC performance: A review

Evaluating electrocatalytic activities of Pt, Pd, Au and Ag-based catalyst on PEMFC performance: A review

Coupled Stacking Faults in Silver Nanorods for CO2 Electroreduction.

The interaction of defects has been proven effective in regulating the mechanical properties of structural materials, while its influence on the physicochemical performance of functional materials has been rarely reported. Herein, we synthesized Ag nanorods with dense stacking faults and investigated how the defect interaction affects the catalytic properties. We found that the stacking faults can couple with each other to form a unique structure of opposite atoms with extortionately high tensile strain. Experimental and theoretical analyses reveal that the opposite-atom structure facilitates the adsorption and activation of CO2 molecules, thus improving the catalytic performance of the carbon dioxide electroreduction reaction (CO2RR). As a result, Ag nanorods achieve high CO partial current density (-11.87 mA cm-2 at -0.8 V vs RHE) and high Faraday efficiency (>95%), superior to most Ag-based catalysts. Our work indicates that the defect interaction is an effective means to boost the performance of functional materials.

Study on the effect and mechanism of support structure and characteristic on Ag-based catalysts for low-temperature selective catalytic oxidation of ammonia

Study on the effect and mechanism of support structure and characteristic on Ag-based catalysts for low-temperature selective catalytic oxidation of ammonia

Oxygen reduction reaction on Ag nanocatalysts prepared by the microemulsion method

Oxygen reduction reaction on Ag nanocatalysts prepared by the microemulsion method

Modulating Silver Performance in Electrocatalytic Oxidation of HCHO via SMSI between Ag-Co3O4 Interfaces.

The replacement of oxygen evolution reactions with organic molecule oxidation reactions to enable energy-efficient hydrogen production has been a subject of interest. However, further reducing reaction energy consumption and releasing hydrogen from organic molecules continue to pose significant challenges. Herein, a strategy is proposed to produce hydrogen and formic acid from formaldehyde using Ag/Co3O4 interface catalysts at the anode. The key to improving the performance of Ag-based catalysts for formaldehyde oxidation lies in the strong SMSI achieved through the well-designed "spontaneous redox reaction" between Ag and Co3O4 precursors. Nano-sized Ag particles are uniformly dispersed on Co3O4 nanosheets, and electron-deficient Agδ+ are formed by the SMSI between Ag and Co3O4. Ag/Co3O4 demonstrates exceptional formaldehyde oxidation activity at low potentials of 0.32V versus RHE and 0.65V versus RHE, achieving current densities of 10 and 100mA cm-2, respectively. The electrolyzer "Ag/Co3O4||20% Pt/C" achieves over 195% hydrogen efficiency and over 98% formic acid selectivity, maintaining stable operation for 60 hours. This work not only presents a novel approach to precisely modulate Ag particle size and interface electronic structure via SMSI, but also provides a promising approach to efficient and energy-saving hydrogen production and the transformation of harmful formaldehyde.

Insight into the unique role of silver single-atom in atomic-thickness ZnIn2S4/g-C3N4 Van der Waals heterojunction for photocatalytic hydrogen evolution

The construction of ultra-close 2D atomic-thickness Van der Waals heterojunctions with high-speed charge transfer still faces challenges. Here, we synthesized single-layer ZnIn2S4 and g-C3N4, and introduced silver single atoms to regulate Van der Waals heterojunctions at the atomic level to optimize charge transfer and catalytic activity. At the atomic scale, the impact of detailed structural differences between the two characteristic surfaces of ZnIn2S4 ([Zn-S4] and [In-S4]) on catalytic performance has been first proposed. Experiments combined with the DFT study demonstrate that single atom Ag not only acts as a charge transfer bridge but also regulates the energy band and intrinsic catalytic activity. Benefiting from the enhanced electron delocalization, the synthesized catalyst ZIS/Ag@CN exhibits excellent photocatalytic performance, with a hydrogen production rate of 5.50mmol·g-1·h-1, which is much higher than the reported Ag-based single-atom catalysts so far. This work provides a new understanding of atomic-level heterojunction interface regulation and modification.

Design a well-dispersed Ag-based/CoFe2O4–CNT catalyst for hydrogen production via NaBH4 hydrolysis

Design a well-dispersed Ag-based/CoFe2O4–CNT catalyst for hydrogen production via NaBH4 hydrolysis

Promoting effect of Cu as electron transfer medium on NH3-SCO reaction in asymmetric Ag-Ov-Ti-Sm-Cu ring active site

Selective catalytic oxidation of ammonia (NH3-SCO) has become an effective method to reduce ammonia (NH3) emissions, and is a key part to solve the problem of NH3 pollution. Nevertheless, the optimization of this technology's performance relies heavily on innovation and the development of catalyst design. In this study, a SmCuAgTiOx catalyst with an asymmetric Ag-Ov-Ti-Sm-Cu ring active site was prepared and applied to the NH3-SCO reaction. The low conversion of Cu-based catalysts in NH3 at low temperature and the inherent low N₂ selectivity of Ag-based catalysts were solved. The successful creation of the asymmetric ring active site improved the catalyst's reduction performance. Additionally, Cu, acting as an electron transfer medium, plays a crucial role in enhancing electron transfer within the asymmetric ring active site, thus increasing the redox cycle of the catalyst during the reaction. In addition, some lattice oxygen is lost in the catalyst, resulting in the formation of a large number of oxygen vacancies. This process stimulates the adsorption and activation of surface-adsorbed oxygen, facilitating the conversion of NH3 to an amide (NH2) intermediate during the reaction and reducing non-selective oxidation. The N2 selectivity was improved without significantly affecting the performance of Ag-based catalyst. In-situ diffuse reflectance fourier transform infrared spectroscopy (In-situ DRIFTS) analysis reveals that the SmCuAgTiOx catalyst primarily follows an "internal" selective catalytic reduction (iSCR) mechanism in the NH3-SCO reaction, complemented by the imide mechanism. The asymmetric Ag-Ov-Ti-Sm-Cu ring active site developed in this study provides a new perspective for efficiently solving NH3 pollution in the future.

Promoting Electrochemical Nitrate Reduction to Ammonia on Silver Nanocrystals Doped with Iron Series Elements.

Electrochemical nitrate reduction to ammonia (NRA) is a promising approach to remove environmental pollutants while producing green NH3 under ambient conditions. Ag-based nanomaterials have been used in NRA but their iron series elements (Fe, Co, Ni) doping has not been explored yet. Herein, an effective and versatile doping strategy of Ag nanocrystals by iron series elements for efficient NRA is presented. Experimental results show that doping with Fe, Co or Ni can improve the NRA activity. Among the catalysts, AgCo delivers the best performance with a Faraday efficiency (FE) of 88.3 % and ammonia selectivity of 97.4 % at-0.23 V vs RHE, which is 1.9 and 6.2 times higher than that of plain Ag (46.4 % FE and 15.8 % selectivity), respectively. A highest NO3 - conversion rate of AgCo (91.8 %) is achieved, which maintains 16.4 ppm NO3 --N in 4 hours, meeting the drinking water level (~15 ppm NO3 --N). Moreover, the FE, selectivity, conversion rate of AgCo do not decay after the four consecutive cycles. It is found that Co doping can effectively induce the change of Ag d-band center for optimized NRA. This work reveals doping effects of iron series elements on Ag-based catalysts, and shows potential practical application in NRA.

Design Strategies for High-Performance NH3-SCO Catalysts: Identifying and Modulating Direct Anchoring Sites for Ag on TiO2.

Ammonia (NH3) slip from diesel vehicle aftertreatment systems and internal combustion engines fueled by NH3 or NH3/H2 poses serious environmental problems. Ag-based catalysts are widely used for the selective catalytic oxidation of NH3 to N2 (NH3-SCO), and their performance is greatly dependent on the state of Ag, which is influenced by the anchoring sites on the support. Despite efforts to identify the direct anchoring sites of metal atoms on TiO2, conflicting views persist. Here, we compared the correlation between Ag dispersion and the content of hydroxyl (OH) groups or defects on TiO2 and conducted density functional theory (DFT) calculations, and the results confirmed that the surface OH groups of TiO2 serve as the direct anchoring sites for Ag. By modulating the OH group content through thermal induction, the optimal OH group content on TiO2-800 resulted in more metallic Ag nanoparticles (Ag0 NPs) in larger sizes, leading to the development of an excellent NH3-SCO catalyst. Moreover, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), kinetic studies, and DFT calculations suggested that more Ag0 NPs in larger sizes on 10Ag/TiO2-800 were conducive to O2 activation and NH3 dissociation. Our findings provide new insights for designing efficient NH3-SCO catalysts, and OH groups as direct anchoring sites could be extended to other metals and supports for the rational design of catalysts.

Modulating the Electrocatalytic CO2-CO Performance by Ag Morphology

Highly selective conversion of CO2 into CO molecules remains a major challenge in electrocatalytic CO2 reduction reactions, and metallic silver-based materials have great potential. However, the selectivity and activity of traditional silver (Ag)-based materials cannot reach the desired level, and the development of new Ag-based materials has become a hot research topic. Here, novel ag-glomerated spore-shaped Ag nanomaterials are reported for the efficient reduction of CO2 to CO. The unique nanostructures endowed with larger specific surface area, and the spore-like dispersed Ag nanoparticles (NPs) have more unsaturated Ag sites, which endowed the catalysts with higher intrinsic activity. Electrochemical tests show that spore-like Ag can obtain a Faraday efficiency (FE) of 95.6% at −1 V vs RHE, which is much higher than that of Ag nanowires (NWs) (73%) and ordinary Ag NPs (83%) synthesized in the same period. By using the three different morphologies of Ag synthesized as a research platform and statistically comparing the FE in the corresponding voltage interval, we obtained the influence of morphology effect on the selectivity of CO product production by electrocatalytic CO2 production over Ag-based catalysts, which can be further used as a guideline for catalyst development.

Asymmetric Local Electric Field Induced by Dual Heteroatoms on Copper Boosts Efficient CO2 Reduction Over Ultrawide Potential Window.

Electrocatalytic reduction of CO2 powered by renewable electricity provides an elegant route for converting CO2 into valuable chemicals and feedstocks, but normally suffers from a high overpotential and low selectivity. Herein, Ag and Sn heteroatoms were simultaneously introduced into nanoporous Cu (np-Ag/Sn-Cu) mainly in the form of an asymmetric local electric field for CO2 electroreduction to CO in an aqueous solution. The designed np-Ag/Sn-Cu catalyst realizes a recorded 90 % energy efficiency and a 100 % CO Faradaic efficiency over ultrawide potential window (ΔE=1.4 V), outperforming state-of-the-art Au and Ag-based catalysts. Density functional theory calculations combined with in situ spectroscopy studies reveal that Ag and Sn heteroatoms incorporated into Cu matrix could generate strong and asymmetric local electric field, which promotes the activation of CO2 molecules, enhances the stabilization of the *COOH intermediate, and suppresses the hydrogen evolution reaction, thus favoring the production of CO during CO2RR.

Lattice-confined Ag over MnCoLDH accelerated catalytic oxidation of formaldehyde at ambient temperature: The novel pathway with different oxygen species

Lattice-confined Ag over MnCoLDH accelerated catalytic oxidation of formaldehyde at ambient temperature: The novel pathway with different oxygen species

Capture of single Ag atoms through high-temperature-induced crystal plane reconstruction

The “terminal hydroxyl group anchoring mechanism” has been studied on metal oxides (Al2O3, CeO2) as well as a variety of noble and transition metals (Ag, Pt, Pd, Cu, Ni, Fe, Mn, and Co) in a number of generalized studies, but there is still a gap in how to regulate the content of terminal hydroxyl groups to influence the dispersion of the active species and thus to achieve optimal catalytic performance. Herein, we utilized AlOOH as a precursor for γ-Al2O3 and induced the transformation of the exposed crystal face of γ-Al2O3 from (110) to (100) by controlling the calcination temperature to generate more terminal hydroxyl groups to anchor Ag species. Experimental results combined with AIMD and DFT show that temperature can drive the atomic rearrangement on the (110) crystal face, thereby forming a structure similar to the atomic arrangement of the (100) crystal face. This resulted in the formation of more terminal hydroxyl groups during the high-temperature calcination of the support (Al-900), which can capture Ag species to form single-atom dispersions, and ultimately develop a stable and efficient single-atom Ag-based catalyst.

Insight into the size-dependent activity in Ag/SiO2 catalyzed hydrogenation of dimethyl oxalate to methyl glycolate

Insight into the size-dependent activity in Ag/SiO2 catalyzed hydrogenation of dimethyl oxalate to methyl glycolate

Temperature-driven dynamic evolution process of Ag species on silver-loaded Zr0.2Sn0.8O2 catalyst for selective catalytic oxidation of ammonia

Temperature-driven dynamic evolution process of Ag species on silver-loaded Zr0.2Sn0.8O2 catalyst for selective catalytic oxidation of ammonia

Modulating the anchoring states of Ag on TiO2 by SiO2 to boost the NH3-SCO activity over Ag-based catalysts

Modulating the anchoring states of Ag on TiO2 by SiO2 to boost the NH3-SCO activity over Ag-based catalysts

MOCHAs: An Emerging Class of Materials for Photocatalytic H2 Production.

Production of green hydrogen (H2) is a sustainable process able to address the current energy crisis without contributing to long-term greenhouse gas emissions. Many Ag-based catalysts have shown promise for light-driven H2 generation, however, pure Ag-in its bulk or nanostructured forms-suffers from slow electron transfer kinetics and unfavorable Ag─H bond strength. It is demonstrated that the complexation of Ag with various chalcogenides can be used as a tool to optimize these parameters and reach improved photocatalytic performance. In this work, metal-organic-chalcogenolate assemblies (MOCHAs) are introduced as effective catalysts for light-driven hydrogen evolution reaction (HER) and investigate their performance and structural stability by examining a series of AgXPh (X=S, Se, and Te) compounds. Two catalyst-support sensitization strategies are explored: by designing MOCHA/TiO2 composites and by employing a common Ru-based photosensitizer. It is demonstrated that the heterogeneous approach yields stable HER performance but involves a catalyst transformation at the initial stage of the photocatalytic process. In contrast to this, the visible-light-driven MOCHA-dye dyad shows similar HER activity while also ensuring the structural integrity of the MOCHAs. The work shows the potential of MOCHAs in constructing photosystems for catalytic H2 production and provides a direct comparison between known AgXPh compounds.

Edge-site selective decoration of silver nanoparticles on TiO2 nanosheets for the rapid catalytic reduction of nitroarenes

Edge-site selective decoration of silver nanoparticles on TiO2 nanosheets for the rapid catalytic reduction of nitroarenes

Efficient electroreduction of CO2 to CO on silver single-atom catalysts: Activity enhancement through coordinated modulation of polyaniline

Efficient electroreduction of CO2 to CO on silver single-atom catalysts: Activity enhancement through coordinated modulation of polyaniline