Non-noble CuO-CeO.SUB.2./Nb.SUB.2.O.SUB.5 .catalysts for low-temperature oxidation of carbon monoxide
12403456 ยท 2025-09-02
Assignee
Inventors
Cpc classification
B01J37/0236
PERFORMING OPERATIONS; TRANSPORTING
International classification
B01J23/847
PERFORMING OPERATIONS; TRANSPORTING
B01J37/02
PERFORMING OPERATIONS; TRANSPORTING
Abstract
There is disclosed a highly efficient and economical catalyst for carbon monoxide (CO) oxidation at low temperatures, using a non-noble transition metal composition of copper oxide (CuO), cerium oxide (CeO.sub.2), and niobium oxide (Nb.sub.2O.sub.5). The catalyst, designated as 10CuCeNb, is synthesized via the wet impregnation method and is composed of with 10% CuOCeO.sub.2 supported on Nb.sub.2O.sub.5. It shows a significantly improved performance with full CO conversion achieved at relatively low temperature of 150 C. It demonstrates high stability over a 12-hour reaction time. The activation energy (Ea) is 23.1 kJ mol.sup.1, supporting low-temperature CO oxidation with minimal energy input. The catalyst's high activity and stability are attributed to the formation of oxygen vacancies and active Lewis acid sites generated from the synergistic interaction between CuO, CeO.sub.2, and Nb.sub.2O.sub.5. This catalyst offers a cost-effective alternative to noble metal catalysts for use in catalytic converters, effectively reducing CO emissions in industrial and environmental applications.
Claims
1. A method for catalytic oxidation of carbon monoxide (CO) to carbon dioxide (CO.sub.2), comprising: providing a non-noble catalyst, designated as 10CuCeNb, composed of 10 weight % of Copper oxide (CuO)-Cerium oxide (CeO.sub.2) precursors, supported on Niobium oxide (Nb.sub.2O.sub.5); calcining the non-noble catalyst 10 CuCeNb in the presence of a flow of 50 ml/min of zero air to remove impurities and covert the precursors into their oxide forms exposing a CO containing gas stream to the calcined non-noble catalyst 10 CuCeNb composition at a temperature as low as 150 C.; and oxidizing the CO to CO.sub.2, wherein the catalyst exhibits enhanced activity due to synergistic interaction between the Copper oxide (CuO)-Cerium oxide (CeO.sub.2) i.e., CuO-doped CeO.sub.2 and the Nb.sub.2O.sub.5, and achieves complete CO oxidation at a temperature of 150 C.
2. The method of claim 1, wherein the CO containing gas stream comprises 10 vol. % CO and 20 vol. % Oxygen (O.sub.2) with the balance being argon (Ar), used in a continuous-flow fixed-bed reactor system.
3. The method of claim 2, wherein the catalyst exhibits an activation energy (Ea) of 21.3 kJ mol.sup.1, supporting CO oxidation at a temperature as low as 150 C. or with energy input of 23.1 kJ.Math.mol.sup.1.
4. The method of claim 3, wherein the catalyst maintains stability and consistent CO conversion rates for at least 12 hours.
5. The method of claim 4, wherein CO oxidation follows the Mars-van Krevelen (MvK) mechanism route, wherein CO molecules chemisorb on the catalyst interface to form Cu-carbonyl species that are oxidized to CO.sub.2 by lattice oxygen and an oxygen vacancy (O.sub.v) thereby created in the lattice is subsequently filled by adsorbed oxygen, enabling continuous CO.sub.2 formation.
6. The method of claim 5, wherein the synergistic interaction between the CuOCeO.sub.2 and the niobium oxide support creates a solid solution that generates oxygen vacancies, thereby enhancing catalytic activity.
7. The method of claim 6, wherein doping the copper oxide into the cerium oxide, disrupts charge balance within the ceria lattice to create oxygen vacancies, that serve as active sites for adsorption and activation of the CO molecules.
8. The method of claim 7, wherein the niobium oxide enhances redox characteristics and develops active acidic sites (Lewis acid sites) upon incorporation with the CuO and the CeO.sub.2, thereby generating oxygen vacancies for CO adsorption and oxidation.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
(1) The subject matter that is regarded as the invention is particularly pointed out and distinctly claimed in the claims at the conclusion of the specification. The foregoing and other aspects, features, and advantages of the invention are apparent from the following detailed description taken in conjunction with the accompanying drawings in which:
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DETAILED DESCRIPTION OF THE INVENTION
(7) The aspects of the proposed non-noble transition metal catalyst 10CuCeNb for low-temperature CO oxidationaccording to the present invention will be described in conjunction with
(8) The present invention introduces a catalyst composed of non-noble transition metals comprising copper oxide (CuO), cerium oxide (CeO.sub.2), and niobium oxide (Nb.sub.2O.sub.5) to be used in catalytic converters for efficient oxidation of carbon monoxide (CO). The catalytic converter aims to transform harmful carbon monoxide (CO) into less harmful compounds through catalytic oxidation reactions. Notably, the catalyst exhibits high activity, especially at low temperatures, enabling efficient conversion of carbon monoxide (CO) into less harmful carbon dioxide (CO.sub.2) at these lower temperatures. In an embodiment of the present invention, the CuOCeO.sub.2/Nb.sub.2O.sub.5 catalyst formulation achieves total/complete oxidation at a relatively low temperature of 150 C. The invention leverages affordable and readily available non-noble metals (copper, cerium, and niobium) instead of expensive and scarce traditional noble metals (such as platinum and palladium) for catalytic oxidation. It thereby offers an efficient sustainable and economically viable alternative for effectively mitigating pollution due to CO emissions.
(9) In a specific embodiment of the invention, the non-noble catalyst, designated as 10CuCeNb, has a formulation composed of 10 weights percent of CuOCeO.sub.2 supported on Nb.sub.2O.sub.5. It is synthesized via the wet impregnation method using CuOCeO.sub.2 precursors supported on niobium oxide with varying loading levels. The synergistic interaction between cerium oxide, copper oxide, and niobium oxide creates a solid solution that generates oxygen vacancies, thereby enhancing the catalytic activity of 10CuCeNb. This catalyst endures high stability over a long reaction time, demonstrates high selectivity, and high activity for CO oxidation reaction at low temperature conditions. It has a low activation energy of Ea=21.3 kJ mol.sup.1, allowing CO oxidation to occur at lower temperatures or with less energy input and the kinetics parameters reveal that the fitted activation energy (23.1 kJ mol.sup.1) inversely follows the CO activity trends. The catalyst achieves full CO conversion at temperatures as low as 150 C. It remains stable over time under the reaction conditions and maintains a consistently high CO conversion rate throughout a 12-hour time-on-stream experiment at 150 C. Its activity and stability are sustained regardless of the presence or absence of water in the feed.
(10) The significance of the invention lies in the development of a CuOCeO.sub.2/Nb.sub.2O.sub.5 catalyst that enables low-temperature catalytic processes that attains full oxidation and using non-noble transition metals as the active components. This catalyst is developed using non-noble metal oxides consisting of copper oxide and cerium oxide supported on niobium oxide, which are much more affordable and readily available compared to noble metals like platinum and palladium, which are of high cost and limited availability. As a CO oxidation catalyst, it is engineered to possess a variety of desirable physicochemical properties, including a wide operating temperature range, no need for pre-use activation, the capability for regeneration, and an extended lifespan. The significant activity exhibited by the catalyst, achieving total CO oxidation at relatively low temperature of 150 C., makes it a feasible solution for converting CO to CO.sub.2. The enhanced catalytic activity is attributed to the synergistic interaction between cerium oxide, copper oxide, and niobium oxide, which results in the formation of a solid solution closely associated with the generation of oxygen vacancies and active sites. Furthermore, the CuOCeO.sub.2/Nb.sub.2O.sub.5 catalyst exhibits long-term stability under operating conditions, ensuring durability and consistent performance over time. It resists deactivation when exposed to CO.sub.2 and H.sub.2O in the feed gas stream or under high CO loads. This resistance to deactivation is a significant advantage over noble metal-based catalysts such as Au, Pt, Rh, Pd, which, despite their higher catalytic activity, suffer from rapid deactivation under high CO loads due to significant amount of CO adsorption on the surface of the noble metal that can poison the catalyst. Other transition metal oxides like cobalt, nickel, manganese, and iron oxides, are also unstable and prone to deactivation when exposed to CO.sub.2 and H.sub.2O in the feed gas stream. Thus, the 10CuCeNb catalyst offers a cost-effective, efficient, and stable solution for catalytic converters, addressing both economic and environmental concerns.
(11) The 10CuCeNb catalyst discussed herein can be employed in catalytic converters to mitigate harmful gases that threaten human health, such as carbon monoxide (CO). These converters transform CO into less harmful compounds through low-temperature catalytic processes. This invention offers several notable benefits: 1) Cost-Effectiveness: The 10CuCeNb is a cost-effective alternative to noble metal catalysts for catalytic converters. This approach addresses the cost factor associated with noble metals, significantly reducing the overall cost of catalytic converters, which is largely influenced by the cost of the catalyst itself. 2) High Efficiency: The catalyst is highly efficient, achieving total oxidation of CO at temperatures as low as 150 C., which demonstrates its feasibility for CO oxidation to CO.sub.2. 3) Stability and Durability: The 10CuCeNb catalyst maintains high stability and consistent performance over extended periods, which is crucial for practical industrial applications. Its durability under real operating conditions ensures reliable long-term use. Given these advantages, the 10CuCeNb catalyst is highly suitable for the development of catalytic converters and underscores its potential for long-term use in catalytic applications. It can be applied in the manufacturing of catalytic converters for vehicles, energy industries, and heating systems to reduce CO emissions as well as by companies offering environmental solutions. Its effectiveness and sustainability in reducing CO emissions make it ideal for mitigating pollution across various industrial applications and the automobile industry.
(12) In an embodiment of the present invention, transition metals such copper with low valence ions is introduced through doping into Cerium oxide (CeO.sub.2). Cerium oxide plays a vital role in providing high oxygen storage capacity and creating oxygen vacancies, which are crucial for CO oxidation. Doping CeO.sub.2 with low valence ions disrupts the charge balance within the ceria lattice structure. This disruption leads to the creation of oxygen vacancies or surface defects within the ceria lattice, which are essential for CO oxidation. These vacancies serve as active sites for the adsorption and activation of CO molecules, facilitating their conversion into less harmful compounds. Incorporation of CuO and CeO.sub.2 into niobium species creates highly distorted octahedrally coordinated NbO.sub.6 species. These species that act as Lewis acid sites, form NbOCe bonds, and generate substantial number of oxygen vacancies crucial for CO oxidation. CO molecules chemisorb on the catalyst interface during oxidation, forming Cu-carbonyl species that are oxidized to CO.sub.2 by lattice oxygen, following the Mars-van Krevelen (MvK) mechanism route. Cu-carbonyl species being oxidized by the interface lattice oxygen, leaves an oxygen vacancy (Ov) that is then filled by adsorbed oxygen, which can react with another carbonyl species, allowing continuous CO.sub.2 formation.
(13) Cerium oxide and copper oxide are selected as key components of the catalyst due to their advantageous properties. Cerium as a catalyst is highly effective in various applications, including CO oxidation, the water-gas shift reaction, and hydrocarbon conversion. Cerium oxide has garnered significant interest among non-precious metal catalysts due to its exceptional oxygen storage capacity. This capacity stems from its ability to switch between Ce.sup.4+ and Ce.sup.3+ cations, enabling the redox couple to transform readily and generate oxygen vacancies within the lattice. These vacancies prevent the sintering of the supported metal or metal oxide phase by creating robust surface bonding interactions. However, pure ceria has poor thermal stability. Incorporating metals or metal oxides into its crystal structure can enhance its activity and thermomechanical properties. These incorporated elements can improve electron transfer rates by influencing surface structure and adsorption site acidity. The introduction of transition metals through doping into CeO.sub.2 can create oxygen vacancies or surface defects within the ceria lattice, which are crucial for CO oxidation. Mixed metal oxides have received more attention mainly because of their improved mechanical stability, selectivity, and reducibility. Doping of CuO/CeO.sub.2 catalysts is particularly active for full CO oxidation, with activity several orders of magnitude higher than traditional Cu-based catalysts and comparable or superior to Pt-based catalysts. Well-dispersed Cu over ceria catalysts has shown effective performance for CO oxidation both in the presence and absence of hydrogen. The co-precipitation method has been reported for synthesizing copper oxide supported on CeO.sub.2 catalysts. The initial step in preparing any catalyst with high activity and ease of preparation involves selecting the appropriate synthesis method. This disclosure employs the wet impregnation method, involving calcination at high temperatures. The highest activity is achieved when the catalyst is calcined at a very high temperature because a highly stable CuCeO.sub.2 solid solution is formed. Particularly, the CO oxidation activity of copper oxide supported on cerium oxide exceeds that of Pt/Al.sub.2O.sub.3. The CuOCeO.sub.2 system demonstrates high activity due to the development of sites at their interface where CO can easily extract oxygen to create CO.sub.2. A major issue with CuO/CeO.sub.2 system catalysts is the high cost of ceria, which the present invention addresses by using niobium oxide.
(14) In an embodiment of the present disclosure, Niobium is another trace element that has been used as a support in catalytic process. Niobium oxides serve as an excellent catalytic promoter in heterogeneous processes. The impact of Nb-incorporated catalysts that is found to be most significant is the enhanced redox characteristics and the development of active acidic sites which boost the activity of catalyst. While cerium oxide is commonly used as a catalyst support, we opted for niobium oxide as a more cost-effective alternative. Niobium oxide offers similar benefits to cerium oxide but at a lower cost, making it a more practical choice for large-scale applications.
(15) In an embodiment of the present invention, the specific preparation method of the catalyst involves the wet impregnation technique with varying loading levels, wherein pre-determined amount of copper and cerium oxides are combined with a pre-determined mass of niobium oxide in a controlled manner to form a slurry, followed by calcination. The wet impregnation method is used as an appropriate method in preparing the catalyst with high activity and ease of preparation. In another embodiment of the invention, the wet impregnation method involves combining 10 weights % of CeO.sub.2 and copper precursor to create a solution. This solution is then carefully added dropwise to a predetermined mass of niobium oxide until a slurry-like mixture is formed. The mixture is stirred at 70 rpm and maintained at 30 C. for 1 hour before being placed in an oven at 105 C. overnight. Subsequently, the catalyst 10CuCeNb undergoes calcination at 500 C. for 4 hours in the presence of a flow of 50 ml/min of zero air to remove impurities and convert the precursors into their oxide forms.
(16) In an embodiment of the invention, the effectiveness of the catalyst is assessed by measuring the catalytic activity and performance of 10CuCeNb in CO oxidation. The effectiveness of catalysts depends on their ability to achieve the desired outcomes of converting CO to CO.sub.2, which in turn, reflects its feasibility in practical applications. To assess the catalytic performance for CO oxidation, experiments are conducted using a continuous-flow fixed-bed reactor system at 1 atm pressure over a temperature range of 100-600 C. The reactor configuration comprises a quartz tube placed within a temperature-controlled electric vertical furnace in which mass of 0.5 g of the prepared catalyst is supported by two quartz wool plugs within the reactor. The feed stream consists of 10 vol. % CO, 20 vol. % O.sub.2, and the remaining balance of Ar. The feed stream is adjusted to a total flow rate of 150 cm.sup.3 min using digital mass flow controllers. Product analysis is performed using an online gas chromatograph (such as GC-TCD). The CO conversion under steady state was calculated by the given Equation (1):
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Where X % denotes the percentage conversion of CO, and outlet and inlet concentrations of CO are represented as [CO].sub.out and [CO].sub.in respectively. Notably, the developed catalysts demonstrate high activity, achieving complete CO conversion (total oxidation) to CO.sub.2 at a relatively low temperature of 150 C. The synergistic interaction between cerium oxide, copper oxide and niobium oxide results in the formation of a solid solution closely associated with the generation of oxygen vacancies and active sites, thereby enhancing the activity of the catalysts. In another embodiment of the invention, the catalytic activity is confirmed through various characterization analyses conducted on the developed catalysts.
(18) In an embodiment of the present invention, the stability of the developed catalyst is assessed. The practical utilization of a catalyst in industries heavily relies on its ability to maintain stability under real operating conditions and consistent performance over time. In one embodiment, a 12-hour time-on-stream experiment is conducted to evaluate the long-term stability of the developed catalyst at 150 C., under identical conditions and feed composition for 12 hours. The CO conversion rate per hour is measured to evaluate stability. The CO conversion rate remains nearly constant and high throughout the entire 12-hour duration, indicating stable performance over time. This observation highlights the catalyst's exceptional stability and suitability for long-term use in catalytic converters.
(19) The developed catalyst as proposed here, demonstrates high activity in achieving full oxidation of CO at a relatively low temperature in the catalytic activity test. These findings are validated in another embodiment of the invention, using kinetic values. The kinetics values are calculated, including the rate of reaction and activation energy, to verify the activity of the developed catalyst. The 10CuCeNb catalyst exhibits the lower activation energy of Ea=21.3 kJ mol.sup.1, enabling the CO oxidation reaction to occur at lower temperatures or with less energy input. In different embodiments of the present disclosure, various characterization analyses of the catalyst are conducted for comprehending the physiochemical properties of the prepared catalysts and their effect on the desired catalytic activity. The analyses comprise employing various techniques such as X-ray diffraction (XRD), Fourier transform infrared (FT-IR), Transmission electron microscopy (TEM), combined Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements and density-functional theory (DFT) computations which confirm the interaction of niobium oxide and cerium oxide that cause the high activity within the low temperature range during the oxidation mechanism.
(20) The FTIR spectra of the prepared samples confirm the incorporation of CuO and CeO.sub.2 into the niobium species. This incorporation results in the creation of highly distorted octahedrally coordinated NbO.sub.6 species. These species serve as Lewis acid sites and promote the formation of NbOCe bonds, generating a substantial number of oxygen vacancies crucial for the CO oxidation process.
(21) In an embodiment of the present invention, DRIFTS analysis is conducted to investigate the mechanism of CO adsorption on catalyst surface. The CO adsorption on catalyst surface follows the Mars-van Krevelen (MvK) mechanism route, as confirmed by in situ DRIFTs analysis. In a further embodiment of the invention, the DFT computations demonstrate the mechanisms for the oxidative transformation of CO into CO.sub.2. The CO molecules chemisorb on the interface of the prepared catalyst, leading to the formation of Cu-carbonyl species. These species are subsequently oxidized by the interface lattice oxygen, resulting in CO.sub.2 species, and leaving an oxygen vacancy (O.sub.v) at the interface. Finally, the oxygen vacancy is filled by adsorbed oxygen, which can react with another carbonyl species, allowing continuous CO.sub.2 formation.
(22) The present solution addresses the development of a cost-effective catalyst with high activity and selectivity for the CO oxidation reaction, both in the presence and absence of H.sub.2O in the feed stream, under low-temperature conditions. In an embodiment of the proposed solution, ceria and niobium oxide doped with CuO, and precursors of CuOCeO.sub.2 supported on niobium oxide with different loadings, are prepared using the wet impregnation method. These prepared samples are subsequently tested for CO oxidation, and a comparative study of their activity is conducted. In this regard, different Cu-doped ceria and niobium-supported catalysts are prepared, characterized, and tested for the reaction. The desired catalysts are prepared using the wet impregnation method as detailed elsewhere. The procedures for preparing niobium oxide-supported catalysts are followed, resulting in catalysts denoted as 5CuNb, 10CuNb, and 15CeNb. For mixed oxides of copper oxide and cerium oxide acting as precursors and supported on niobium oxide, appropriate percentages, specifically X % CuOY % CeO.sub.2/(100-(X+Y) % Nb.sub.2O.sub.5 are prepared, where X, Y=5% and 10%, respectively. In the synthesis of all samples, Copper (II) nitrate trihydrate (Cu(NO.sub.3).sub.2.3H.sub.2O), CeO.sub.2 micro-powder, and ammonium niobate (V) oxalate hydrate (C.sub.4H.sub.4NNbO.sub.9) are utilized as precursors for CuO, CeO.sub.2, and Nb.sub.2O.sub.5; respectively. Accordingly, the correct quantities of CeO.sub.2 micro-powder (Sigma-Aldrich, >99%) and copper oxide salt are slowly introduced into a stirring solution of ammonium niobate (V) oxalate hydrate (C.sub.4H.sub.4NNbO.sub.9) solution. This mixture is then dried overnight and undergoes calcination for 4 hours at 400 C. in static air at a flow rate of 100 ml/min. These catalysts are denoted as 5CuCeNb and 10CuCeNb, where the weight percentages of Cu and Ce are 5% and 10%, respectively.
(23) In another embodiment according to the present disclosure, catalytic run experiments are conducted to evaluate the effectiveness and efficiency of the prepared catalysts in oxidizing CO. The carbon monoxide oxidation experiments are carried out in a tubular quartz reactor positioned at the centre of an electrically heated furnace. The temperature range varies from 100 to 400 C., with intervals of 50 C., and the reactor operates at atmospheric pressure. In each experiment, a fixed amount of catalyst (0.5 g) is placed in the middle of the reactor tube and secured using ultra-pure quartz wool. The total flow rate of the feed stream (10% CO, 20% O.sub.2, with the remaining balance of Ar) is 150 cm.sup.3 min.sup.1, adjusted using digital mass flow controllers. The weight hourly space velocity (WHSV) of the reactants is set at 18000 cm.sup.3g.sup.1h.sup.1 for the experiments. The products leaving the reactor are analysed using a Micro GC. In another embodiment, to evaluate the catalyst's performance under moisture conditions, the feed gas is passed through a water vapor saturator at a flow rate of 150 ml/min, maintaining the previously mentioned feed composition. The CO conversion under steady state is calculated by the Equation (1):
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Where X % is the percentage conversion of CO and outlet and inlet concentrations of carbon monoxide are represented as [CO].sub.out and [CO].sub.in respectively. The criteria for the absence of external and internal mass transport resistances are accordingly satisfied. The rate of reaction is calculated by using the below Equation (2) and the activation energy, Ea of the catalysts is estimated by linear fitting of the Arrhenius equation represented as Equation (3):
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where F.sub.CO represents the volumetric flow rate of CO inlet into the feed stream and X.sub.CO denotes the conversion of CO, and W stands for the weight of the catalyst used in the reaction; k denotes the rate constant of the reaction, T the absolute temperature, A is the pre-exponential factor/Arrhenius factor, e is the Euler's number and R the universal gas constant. To estimate the kinetic parameters Ea (activation energy) and rate of the equation, the CO oxidation reaction is carried out within a temperature range of 80-150 C. to keep CO conversion below 15%, using a feed gas composition of 10% CO/20% O.sub.2/Ar.
(27) In an embodiment of the proposed solution, the catalytic activity and reaction kinetics are analyzed. The oxidation of CO over different catalysts is examined, and conversion is measured under the above-mentioned conditions. In all cases, the change in catalytic activity toward CO oxidation is explicit in the percentage of CO conversion as a function of temperature.
(28) In the second case, the catalyst support is changed from cerium oxide to the cheaper alternative of niobium oxide. It is found that increasing the Cu % loading decreases the activity of CO oxidation. Comparing the T.sub.100 values (from
(29) The performance of the catalysts used herein is demonstrated by the CO conversion profile, which compares favourably to previous reports. For instance, a high surface area modified ceria catalyst achieves 50% CO conversion at 320 C. under similar conditions. Similarly, lanthanum-doped ceria and trace metal-doped (M: La and Pr) catalysts exhibit approximately 50% CO conversion at temperatures above 300 C. Additionally, it is observed that the CuOCeO.sub.2 system supported on other oxides, such as Al.sub.2O.sub.3, shows complete CO conversion at temperatures exceeding 200 C. These findings highlight the reasonable performance of the catalysts employed in this disclosure.
(30) In another embodiment of the invention, the stability test is conducted on the prepared catalysts. The industrial application of a catalyst greatly depends on its stability during real operating conditions, highlighting the importance of ensuring its durability and performance over time. Hence, a 12-hour time-on-stream experiment is conducted to examine the long-term stability of the best-performing catalyst, 10CuCeNb, at 150 C.
(31) The high activity and catalytic performance exhibited by the proposed catalyst 10CuCeNb is attributed to the synergistic interaction between cerium oxide, copper oxide, and niobium oxide, which is a key feature that significantly enhances the catalyst's effectiveness. This interaction results in the formation of a solid solution that generates oxygen vacancies, thereby enhancing the catalytic activity. Doping CeO.sub.2 with transition metals that have low valence ions disrupts the charge balance within the lattice structure. To maintain charge neutrality, this disruption leads to the formation of oxygen vacancies or surface defects within the ceria lattice. These vacancies and defects are crucial for CO oxidation, as they enhance the catalyst's ability to adsorb and activate oxygen molecules. These surface defects or oxygen vacancies change the nearby electronic configuration, significantly affecting surface reactivity. According to the Volkenshtein electronic theory, the presence of defect sites associated with oxygen vacancies (O.sub.v) modifies the Fermi energy level. This modification facilitates oxidation processes by making it easier for the catalyst to interact with and oxidize reactant molecules. The altered electronic environment due to these vacancies provides active sites that are more conducive to the adsorption and activation of oxygen, thereby improving the overall catalytic efficiency for CO oxidation. In bare ceria, Ce.sup.4+ is reduced to Ce.sup.3+ by CO, resulting in the formation of an O.sub.v. When the vacancy forms, two excess electrons are left behind and fill the 4f orbitals of Ce.sup.4+, converting it to Ce.sup.3+. The feed gas O.sub.2 then reacts with the solid surface to fill the created oxygen vacancy O.sub.v, a process known as O.sub.2 activation, during which highly active atomic oxygen species are generated. Finally, CO reacts with these highly active atomic oxygen species to form CO.sub.2. According to the disclosure, niobium oxide acts as a support while cerium and copper oxide act as promoters.
(32) To support this key feature, in another embodiment of the present invention, the effects of doping niobium oxide with cerium oxide and copper oxide are investigated. Results reveal a contraction in the lattice constant of the prepared catalysts. This contraction suggests that Nb and Cu nanoparticles have successfully embedded into the ceria matrix after interaction. This embedding is likely due to the substitution of Ce.sup.4+ ions with Nb.sup.5+ or Cu.sup.2+ ions, which have smaller ionic radii. Specifically, niobium has an ionic radius of 0.64 and copper has an ionic radius of 0.72 , both of which are smaller than the ionic radius of cerium, which is 0.97 . The smaller ionic radii of niobium and copper allow them to fit into the ceria lattice, leading to the observed contraction. This synergistic interaction results in the formation of a solid solution, which creates defects closely linked to the generation of oxygen vacancies. These oxygen vacancies facilitate achieving the reaction at lower temperatures. To further confirm these interactions that cause the defects, Raman analysis of pure ceria and the claimed catalyst is conducted to analyse the differences after the incorporation of these nanoparticles.
(33) In another embodiment, O.sub.2-TPD experiments are conducted to analyse the nature of oxygen on the catalyst surface. The active oxygen species present on the catalyst surface are recognized to play a crucial role in enhancing catalytic activity in oxidation reactions.
(34) In conclusion, this disclosure investigates the capability of novel 10% CuOCeO.sub.2/Nb.sub.2O.sub.5 catalysts for low-temperature CO oxidation under atmospheric conditions. In this regard, Ceria and Niobium Oxide doped with Cu and precursors of CuOCeO.sub.2 supported on Niobium Oxide with different loadings are prepared, characterized, and tested for the CO oxidation reaction. Among all the prepared catalysts, 10% CuOCeO.sub.2/Nb.sub.2O.sub.5 shows high CO oxidation activity with full conversion at a relatively low temperature (150 C.) due to the synergistic effects between CuO, CeO.sub.2 and the support Nb.sub.2O.sub.5 while remaining stable over time. The CO conversion of the best-performing catalyst remains relatively stable throughout a 12-hour time-on-stream test in the absence of water in the feed. Additionally, the kinetics parameters determined reveal activation energy (23.1 kJ mol.sup.1) inversely following CO activity trends. This development opens up possibilities for the practical use of affordable and highly efficient catalyst materials in cost-effective technologies to reduce CO emissions. The catalyst is used to convert CO, which poses harmful effects to humans, plants, animals, and the environment, into less harmful CO.sub.2 compounds, thereby reducing CO emissions and mitigating its detrimental impacts. As a cost-effective alternative to expensive noble catalysts, this catalyst offers a sustainable and efficient solution to pollution. The proposed catalyst is particularly applicable in the automotive industry for manufacturing catalytic converters for vehicle exhaust systems. Additionally, it can be employed in various industrial processes that generate toxic gases, including energy-related industries and heating systems, as well as by companies providing environmental solutions.
(35) Benefits of the proposed 10CuCeNb catalyst for CO oxidation in accordance with the present invention include the catalyst offering a cost-effective alternative to noble metal catalysts for catalytic converters, high efficiency by achieving total oxidation of CO at low temperatures as low as 150 C., and high stability and maintenance of performance over extended periods, crucial for catalytic converter development.
(36) Many changes, modifications, variations and other uses and applications of the subject invention will become apparent to those skilled in the art after considering this specification and the accompanying drawings, which disclose the preferred embodiments thereof. All such changes, modifications, variations and other uses and applications, which do not depart from the spirit and scope of the invention, are deemed to be covered by the invention, which is to be limited only by the claims, which follow.