CO2 Activation Research Articles

Self-standing Z-scheme structured heterogeneous nanosheet arrays of ZnIn2S4/cobalt porphyrin sulfonate for bifunctional photocatalytic carbon dioxide reduction and antibacterial

Photocatalytic CO2 reduction for solar fuel generation and photocatalytic sterilization are highly desired green routes for sustainable environmental purification. Herein, a bifunctional self-standing nanosheet array of Z-scheme structured inorganic–organic heterojunction is synthesized via in-situ growth of ZnIn2S4 (ZIS) on carbon cloth (CC) followed by self-assembly with cobalt porphyrin (meso-tetra(4-sulfonatophenyl) porphyrin, CoTPPS). The obtained CC-ZIS-CoTPPS performed well in the photocatalytic CO2 reduction and antibacterial processes simultaneously in a portable photocatalytic system with a negligible amount of solution. Specifically, the optimized CC-ZIS-CoTPPS demonstrates more than 140 times enhanced CO evolution than pristine CoTPPS. Experimental and theoretical results imply that the enhanced photocatalytic CO2 reduction is associated with elevated light absorption, promoted charge separation, and improved CO2 activation in the inorganic–organic Z-scheme heterojunction. In addition, the self-standing nanosheet array possesses a mechanical cutting effect, which can kill bacteria adhering to the surface even in dark conditions. Moreover, CC-ZIS-CoTPPS achieved a 100 % killing rate under visible light irradiation by synergistically chemical and mechanical sterilization. Furthermore, CC-ZIS-CoTPPS exhibits efficient bifunctional photocatalytic photocatalytic CO2 reduction coupled with in-situ sterilization. This work presents an atomic perspective for developing innovative bifunctional photocatalysts, which hold great potential in portable devices to alleviate energy and environmental crises.

Enhancement of CO2 adsorption and oxygen transfer properties on γ-Al2O3 support through surface modification with MgO-ZrO2 for coke suppression over Ni catalyst in CO2 reforming of methane

This work focuses on employing commercial γ-Al2O3 for surface modification with MgO-ZrO2 mixed oxide to enhance the potential of CO2 adsorption and oxygen mobility. This enhancement facilitates its application as a support in catalysts for CO2 utilization such as CO2 reforming of methane (CRM). To achieve this perspective, γ-Al2O3 was modified with 10 wt.% of various MgO and ZrO2 contents (MgO:ZrO2= 10:0, 9:1,7:3, 5:5, 3:7, 1:9 and 0:10) using the impregnation method. All samples including unmodified γ-Al2O3 (Al) were characterized. Due to the increase in basicity and oxygen transfer around the surface, the improvement of the CO2 adsorption was observed on γ-Al2O3 modified with 9 wt.% MgO-1 wt.% ZrO2 (9Mg1ZrAl) and 10 wt.% MgO (10MgAl), respectively. An application of these two superior samples as a support of 10 wt.% Ni (10Ni) catalysts for CRM was investigated and compared with an unmodified γ-Al2O3. Characterization results suggest the formation of NiO-MgO solid solution at the surface due to the decrease in metal-support interaction and the increase in metal dispersion. The Ni catalysts with the surface-modified support show higher CO2 activity that raises carbon deposition resistance. The greatest coke prevention was observed on 10Ni/9Mg1ZrAl that lowers the coke deposition by 42% compared to 10Ni/Al. It indicates that the composition of this modification allowed very low ZrO2 portion to merge with MgO and MgO to form solid solution with NiO. This enables the 10Ni/9Mg1ZrAl catalyst to generate labile oxygens which can be conveyed to the Ni metal sites on the catalyst.

First-principles study of selective CO2 activation to methanol on PdZn/TiO2: Unveiling Zn/Pd ratio on catalysis performance

In this study, a series of Pd(8-n)Znn/TiO2(n=0–8) were investigated via density functional theory (DFT) to understand the influence of Zn/Pd ratio on their catalysis performance of conversion CO2 to methanol. It is revealed that Zn prefers to replace the bottom-layered Pd when its molar concentration in composition increases. For all surface models, interface between cluster and support plays a key role in CO2 stabilization and activation. Increasing Zn/Pd ratio could weaken the binding strength of CO2 over catalyst, which further hinders the “RWGS” pathway while promotes the “Formate” pathway. Based on the calculation results, a Brønsted–Evans–Polanyi (BEP) relation between the activation barrier (Ea) of key elementary steps from both mechanisms and the binding strength of key intermediates has been established, from which the optimum Zn/Pd ratio leading to the best catalysis performance has been determined. Moreover, it is found that water inclusion in the system does not change the Ea of rate-determining step much even though it has a promotion effect on OH formation steps. Overall, this work provides some meaningful insight into the influence of cluster composition on the catalysis performance of PdZn-based catalyst and provides valuable information about rational design of the supported bimetallic catalyst.

Anchoring Ag Atom on Carbon Vacancy Enriched Carbon Nitride to Synergistically Promote CO2 Photoredution with Water

AbstractPristine carbon nitride (CN) has low CO2 reduction ability due to its sluggish charge carriers transfer and CO2 activation. Herein, carbon vacancy (CV) and Ag single atoms (SAs) with N2 coordination are simultaneously introduced into CN with the ordered structure for stable and efficient photoreduction of CO2 in the presence of H2O. The optimal sample loaded with 0.053 wt.% Ag evolve 173.0 µmol g−1 CO in 3 h with 89% selectivity, which is 11.7 times higher than that of pristine CN (14.7 µmol g−1). Experiments and theoretical calculations reveal that the CV and Ag–N2 sites promote CO2 adsorption/activation and the generation of *COOH and *CO. KSCN‐assisted calcination induces more ordered arrangement of melon chains, which can accelerate charge transfer/separation and facilitate H2O oxidation, thus accounting for the largely improved CO2 photoreduction performance. This study adopts a new method to prepare Ag SA‐anchored and C‐deficient CN, and provides insights into their synergistic roles in enhancing CO2 reduction.

Enhanced Local CO Coverage on Cu Quantum Dots for Boosting Electrocatalytic CO2 Reduction to Ethylene

AbstractEthylene (C2H4) electrosynthesis from the electrocatalytic CO2 reduction process holds enormous potential applications in industrial production. However, the sluggish kinetics of C─C coupling often result in low yield and poor selectivity for C2H4 production. Herein, the performance of Cu catalysts of varying sizes is investigated, prepared via a cryo‐mediated liquid phase exfoliation technique, for the electrochemical CO2 reduction to C2H4. The activity and selectivity of C2H4 gradually increase as the size of the Cu catalysts decreases from tens of nanometers to a few nanometers. Impressively, the 5 nm Cu quantum dots (Cu‐5) achieve a maximum C2H4 Faradaic efficiency (FE) of 81.5% and a half‐cell cathodic energy efficiency (CEE) of 42.2% with a large partial current density of 1.1 A cm−2 at −0.93 V versus the reversible hydrogen electrode. Structural characterization and in situ spectroscopic analysis reveal that the Cu‐5 quantum dots, dominated by the (100) facet, provide an abundance of active sites that enhance CO2 adsorption and activation, promoting the formation of *CO intermediates. The accumulation of *CO intermediates on the Cu active sites facilitates the CO‐CHO coupling reaction, thus enhancing the C2H4 production rate.

Mg bulk and surface modification on Ni/Y2Ti2O7 catalyst for dry reforming of methane

Dry reforming of methane (DRM) can simultaneously convert two greenhouse gases, CH4 and CO2, into high value-added synthetic gas, which can effectively alleviate the energy crisis and optimize the human ecological environment. In this work, the effect of Mg addition method on the activity of the Y2Ti2O7 pyrochlore supported Ni catalysts was investigated in DRM. The H2-TPR and XPS results showed that Mg modification enhanced the interaction between Ni and Y2Ti2O7 pyrochlore support. Thus, much smaller Ni grains with better thermal stability could be achieved on the Mg doped Ni/Y2Ti2O7 catalyst, as evidenced by the XRD, H2-TPD and TEM results. CO2-assistant CH4-TPSR demonstrated that Mg surface modification can facilitate the reaction between the activated CO2∗ and the H∗ produced by CH4 dissociation. Mg incorporation increased the basic site of the Ni/Y2Ti2O7 catalyst, as evidenced by CO2-TPD-MS results, which was conducive to the adsorption and activation of CO2 to promote the removal of coke deposition. Consequently, Ni/Y1·5Mg0·5Ti2O7 and Ni–MgO/Y2Ti2O7 catalysts exhibit higher stability and more potent coke resistance than the unmodified Ni/Y2Ti2O7 sample. It is concluded that higher Ni0 dispersion and more mobile active oxygen species are the main reasons for the improvement of activity and coke resistance of the Ni/Y2Ti2O7 catalysts. In addition, in situ DRIFTS results confirmed that CO2 activation of all catalysts followed the formate intermediate species path.

Enhanced leaching control of chromium, antimony, and chlorine utilizing CO2-curing slag-fly ash-based agent

This study strives to address the technical bottleneck posed by leaching risks associated with Cr, Sb, and soluble Cl in low-carbon slag-fly ash-based cementitious materials (BFCM) according to our previous research. The introduction of CO2 activation significantly enhances the dissociation of BFS, leading to superior mechanical performance and environmental safety of BFCM. LT3 matrix of BFCM (BFS: MSWI fly ash: FGDG: cement= 42: 20: 10: 28) showed excellent compressive strength (46.79Mpa at 7d). The LT3 matrix enables effective solidification/stabilization (S/S) of Cr, Sb, and Cl with CO2-curing (7d). Furthermore, the leaching concentrations of Sb and Cl within LT system, exhibit a positive correlation, while they demonstrate a negative correlation with Cr. Sb primarily relies on the levels of Ca2+ and OH- in the leaching solution, critical for the formation and stability of Ca-Sb precipitation based Visual MINTEQ fitting. CO2-curing enhances the S/S efficiency of Cl by accelerating the ion exchange of Cl- with OH- in C-A-H and SO42- in the AFm phase, leading to the formation of functional Friedel’s salt. This process is characterized by OH- dissolution and subsequent CaSO4 crystallization. The LT system activated by CO2 exhibited accelerated reaction kinetics relative to traditional hydration (LH), characterized by rapid BFS dissociation and the formation of functional hydration products such as ettringite, C-(A)-S-H, and Friedel's salt. This process also reduced macropores and capillary pores of BFCM, a positive correlation exists between the relative macropore content and Cl leaching levels, whereas the decrease in both macropores and capillary pores is associated with ettringite crystallization.

CO2 Reduction by Transition‐Metal Complex Systems: Effect of Hydrogen Bonding on the Second Coordination Sphere

AbstractHomogeneous electrocatalysts typified by transition‐metal complex show transcendent potency in efficient energy catalysis through molecular design. For example, metal complexes with elaborate design performed wonderful activity and selectivity for electrocatalytic CO2 reduction. Primary coordination sphere of metal complexes plays a key role in regulating its intrinsic redox properties and catalytic activity. However, the overall reduction efficiency of CO2 is also bound up with the substrate activation process. Transition‐metal complexes are hoped to exhibit reasonable redox potential, reactive activity, and stability, while binding and activating CO2 molecules to achieve efficient CO2 reduction. Construction of second coordination sphere, especially hydrogen‐bonding network of transition‐metal complexes, is reported to be the “kill two birds with one stone” strategy to realize efficient CO2 reduction catalysis via systematic catalyst properties modulation and substrate activation. Herein, we present recent progress on the construction of hydrogen‐bonding network in the second coordination sphere of metal complexes by ligand modification or the introduction of exogenous organic ligand, and the resulted productive enhancement of the catalytic performance of metal complexes by the improvement of adsorption capacity and activation of CO2, proton transfer rate, and stability of reaction intermediates, and so forth.

Enabling Interfacial Lattice Matching by Selective Epitaxial Growth of CuS Crystals on Bi2WO6 Nanosheets for Efficient CO2 Photoreduction into Solar Fuels.

Photocatalytic CO2 reduction serves as an important technology for value-added solar fuel production; however, it is generally limited by interfacial charge transport. To address this limitation, a two-dimensional/two-dimensional (2D/2D) p-n heterojunction CuS-Bi2WO6 (CS-BWO) with highly connected and matched interfacial lattices was designed via a two-step hydrothermal tandem synthesis strategy. The integration of CuS with BWO created a robust interface electric field and provided fast charge transfer channels due to the work function difference, as well as highly connected and matched interfacial lattices. The p-n heterojunctionpromotedelectron transfer from the Cu to Bi sites, leading to coordination of Bi sites with high electronic density and low oxidation state. The Bi sites in BWO nanosheets facilitated the adsorption and activation of CO2, and generation of high-coverage key intermediate b-CO32-, while broad light-harvesting CuS (CS)provide abundant photoinduced electrons that were injected into the conduction band of BWO for CO2 photoreduction reaction. Remarkably, the p-n heterojunction CS-BWO exhibited CO and CH4 yields of 135.7 and 62.5 µmol g-1, respectively, which were significantly higher than those of CS, BWO, and physical mixture CS-BWO nanosheets. This work provided an innovative design strategy for developing high-activity heterojunction photocatalyst for converting CO2into value-added solar fuels.

Ag–Pt Alloy Nanoparticles Modified Zn‐Based Nanosheets for Highly Selective CO2 Photoreduction to CH4

AbstractMulti‐electron involved photoreduction of CO2 to hydrocarbon fuels is a long‐standing challenge, particularly in manipulating the selectivity of the target products. Here, a novel Ag–Pt bimetallic alloy on Zn‐based supports by photo‐deposition is designed for photocatalytic CO2 reduction to CH4 without any additives. This photocatalyst exhibits ≈ 98.9% selectivity for CH4. Experimental and theoretical calculations demonstrated that the excellent performance of the photocatalyst can be attributed to the localized surface plasmon resonance effect of metals, as well as the synergistic effects of the bimetallic sites. These factors are found to be beneficial not only for capturing solar radiation and facilitating electron migration but also for promoting the adsorption and activation of CO2 and the protonation of *CO. As a result, the photocatalyst achieved high selectivity and activity of photoreduction of CO2 to CH4. This work provides insights into the design of photocatalysts with highly selective target products for CO2 reduction.

Covalent Organic Framework Stabilized Single CoN4Cl2 Site Boosts Photocatalytic CO2 Reduction into Tunable Syngas

AbstractSolar carbon dioxide (CO2) reduction provides an attractive alternative to producing sustainable chemicals and fuel. However, the construction of a highly active photocatalyst was challenging because of the rapid charge recombination and sluggish surface CO2 reduction. Herein, a unique Co−N4Cl2 single site was fabricated by loading Co species into the 2,2′‐bipyridine and triazine‐containing covalent organic framework (COF) for CO2 conversion into syngas under visible light irradiation. The resulting champion catalyst TPy‐COF‐Co enabled a record‐high CO production rate of 426 mmol g−1 h−1, associated with the unprecedented turnover number (TON) and turnover frequency (TOF) of 2095 and 1607 h−1, respectively. The catalyst also exhibited favorable recycling performance and widely adjustable syngas production (CO/H2 ratio: 1.8 : 1–1 : 16). A systematical investigation including operando synchrotron X‐ray absorption fine structure (XAFS) spectroscopy, in situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS), and theoretical calculation indicated that the triazine‐based COF framework promoted the charge transfer towards the single Co−N4Cl2 sites that greatly promoted the CO2 activation by lowering the energy barrier of *COOH generation, facilitating the CO2 transformation. This work highlights the great potential of the molecular regulation of COF‐derived single‐atom catalysts to boost CO2 photoreduction efficiency.

Concurrent activation of CO2 and H2O on sulfur-doped CNT-supported nickel phthalocyanine for electrochemical CO2 reduction to CO.

Concurrent activation of CO2 and H2O is essential for CO2 electroreduction reaction, but challenging. A sulfur-doped carbon nanotubes-supported nickel phthalocyanine (NiPc/S-CNTs) can concurrently activate CO2 and H2O, promoting CO2 protonation to *COOH. The NiPc/S-CNTs achieves CO Faraday efficiency of >96% at current density from -20 to -140 mA cm-2.

Mechanism study on the influence of surface properties on the synthesis of dimethyl carbonate from CO2 and methanol over ceria catalysts

The direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol has attracted much attention as an environmentally benign and alternative route for conventional routes. Herein, a series of cerium oxide catalysts with various textural features and surface properties were prepared by the one-pot synthesis method for the direct DMC synthesis from CO2 and methanol, and the structure-performance relationship was investigated in detail. Characterization results revealed that both of surface acid-base properties and the oxygen vacancies contents decreased with the rising crystallinity at increasingly higher calcination temperature accompanied by an unexpectedly volcano-shaped trend of DMC yield observed on the catalysts. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies indicated that the adsorption rate of methanol is slower than that of CO2 and the methanol activation state largely influences the formation of key intermediate. Although the enhanced surface acidity-basicity and oxygen vacancies brought by low-temperature calcination could facilitate the activation of CO2, the presence of excess strongly basic sites on low-crystallinity sample was detrimental to DMC synthesis due to the preferred formation of unreactive mono/polydentate carbonates as well as the further impediment of methanol activation. Moreover, with the use of 2-cyanopyridine as a dehydration reagent, the DMC synthesis was found to be both influenced by the promotion from the rapid in situ removal of water and the inhibition from the competitive adsorption of hydration products on the same active sites.

Direct cleavage of C=O double bond in CO2 by the subnano MoOx surface on Mo2N

Compared to H2-assisted activation mode, the direct dissociation of CO2 into carbonyl (*CO) with a simplified reaction route is advantageous for CO2-related synthetic processes and catalyst upgrading, while the stable C = O double bond makes it very challenging. Herein, we construct a subnano MoO3 layer on the surface of Mo2N, which provides a dynamically changing surface of MoO3↔MoOx (x < 3) for catalyzing CO2 hydrogenation. Rich oxygen vacancies on the subnano MoOx surface with a high electron donating capacity served as a scissor to directly shear the C = O double bond of CO2 to form CO at a high rate. The O atoms leached in CO2 dissociation are removed timely by H2 to regenerate active oxygen vacancies. Owing to the greatly enhanced dissociative activation of CO2, this MoOx/Mo2N catalyst without any supported active metals shows excellent performance for catalyzing CO2 hydrogenation to CO. The construction of highly disordered defective surface on heterostructures paves a new pathway for molecule activation.

Life After Death: Re‐Purposing End‐of‐Life Supercapacitors for Electrochemical Water Desalination

AbstractThis study explores the potential of re‐purposing end‐of‐life commercial supercapacitors as electrochemical desalination cells, aligning with circular economy principles. A commercial 500‐Farad supercapacitor was disassembled, and its carbon electrodes underwent various degrees of modification. The most straightforward modification involved NaOH‐etching of the aluminum current collector to produce free‐standing carbon films. More advanced modifications included CO2 activation and binder‐added wet processing of the electrodes. When evaluated as electrodes for electrochemical desalination via capacitive deionization of low‐salinity (20 mM) NaCl solutions, the minimally modified NaOH‐etched carbon electrodes achieved an average desalination capacity of 5.8 mg g−1 and a charge efficiency of 80 %. In contrast, the CO2‐activated, wet‐processed electrodes demonstrated an improved desalination capacity of 7.9 mg g−1 and a charge efficiency above 90 % with stable performance over 20 cycles. These findings highlight the feasibility and effectiveness of recycling supercapacitors for sustainable water desalination applications, offering a promising avenue for resource recovery and re‐purposing in pursuing environmental sustainability.

Highly stable and electron-rich Ni single atom catalyst for directed electroreduction of CO2 to CO

Transition metal-nitrogen-carbon (M−N−C) are considered as promising candidates for the electrochemical conversion of inert CO2 into high value-added CO products. However, previous reports have focused on Ni single-atom sites (Ni SAs) and the role of Ni nanoparticles (Ni NPs) in CO2 electroreduction reaction (CO2RR) has been overlooked. Herein, we prepared a series of Ni, N-codoped porous carbon (NiNC-T, T represents the temperature) catalysts by combining Ni phthalocyanine pyrolysis and acid etching strategy, which either contain only Ni SAs or both Ni SAs and Ni NPs. Notably, the NiNC-1100 catalyst with both Ni SAs and Ni NPs exhibited 99 % CO faradaic efficiency (FECO) at −0.66 V versus reversible hydrogen electrode (vs. RHE) and FECO above 98 % over a wide potential range (−0.66 V ∼ −1.06 V). Moreover, the FECO of NiNC-1100 remained above 95 % after 100 h of continuous electrocatalysis, which was significantly superior to that of the most advanced Ni single atom electrocatalysts. The systematic characterization results showed that the introduction of Ni NPs can promote the adsorption and activation of CO2 by increasing the electron cloud density of Ni SAs, thus enhancing the CO2RR catalytic performance.

Favorable formation of needle-shaped NiAl2O4 phase over macroporous Ni/CexZr1-xO2–Al2O3 catalysts in one-pot preparation and coke-resistant catalytic performance in dry reforming of methane

In this study, we report the formation of needle-shaped NiAl2O4 via favorable interactions between Ni and Al species over macroporous Ni/CexZr1-xO2–Al2O3 catalysts for dry reforming of methane (DRM) and its remarkable improvement in the catalytic performance. The macroporous catalysts prepared by a one-pot (OP) method promote a favorable interaction between Ni and Al species that results in the formation of unique needle-shaped NiAl2O4 due to easy access to each other compared with that by incipient wetness impregnation. The NiAl2O4 phase in the calcined catalysts transforms into highly dispersed Ni and defective Al2O3 via the Ni exsolution in the reduction step. The presence of oxygen vacancies near Ni0 species facilitates the CO2 activation and enhances the catalyst stability over DRM. The optimized distribution of active sites with abundant defects over macroporous Ni/CexZr1-xO2-Al2O3 catalysts (OP) result in high conversions of CH4 and CO2 and a low coking rate in DRM.

Engineering single-atomic Ni sites stabilized with adjacent spinel nanoparticles to boost CO2 electroreduction

Single-atom catalysts show great potential in the electrochemical CO2 reduction reaction (CO2RR), but face significant challenges in accelerating reaction kinetics. Herein, we develop a three-dimensional heterostructured MgAl2O4/Ni-N-C catalyst via a facile pyrolysis strategy, featuring abundant atomically dispersed Ni sites and ∼14 nm MgAl2O4 nanoparticles. The MgAl2O4 with rich oxygen vacancies is crucial for stabilizing Ni atoms and promoting CO2 activation, thereby contributing to an excellent selectivity of nearly 100 % and good stability for CO production. The CO Faraday efficiency remains > 90 % within a large potential window (−0.57 to −0.97 V vs. RHE), and achieves the maximum of 98.7 % at −0.82 V. Theoretical calculations reveal that MgAl2O4 introduction can modulate the electron structure of Ni atoms, and accelerate the formation of *COOH intermediate, thus boosting CO2RR performance. This research provides a novel approach for the design of high-efficiency single-atom catalysts for CO2 conversion.

A-Site Doping Promotes CO2 Activation and Prolongs Charge Carrier Lifetimes in SrTiO3: Insight from Quantum Dynamics.

Using time-dependent density functional theory and nonadiabatic molecular dynamics, we systematically investigated the effect of A-site doping on the CO2 activation and charge carrier lifetimes in SrTiO3(STO). Our simulations revealed that A-site doping significantly enhances the chemical adsorption of CO2 on SrTiO3 surfaces, which is beneficial for promoting CO2 activation. Moreover, we found that A-site doping can efficiently stabilize the lowest unoccupied molecular orbital (LUMO) of CO2 near the conduction band minimum of STO, promoting the photogenerated electron transfer from the conduction band of STO to the CO2 LUMO. Importantly, A-site doping causes a significant nonadiabatic coupling reduction and prolongs the charge recombination time by a factor of 1.86 compared to the pristine STO. Our study clarifies the influencing mechanism of A-site doping on CO2 activation and charge carrier lifetimes and suggests important principles for the design of high-performance photocatalytic semiconductors.

Boosted Solar Thermochemical Low-Temperature CO2 Splitting On Pt/CeO2 by Interface Catalysis.

Solar thermochemical CO2 splitting using metal oxides is considered as a promising approach to produce solar fuels since it is capable to tap abundant sunlight directly and store solar energy in the renewable fuel. It remains a grand challenge to achieve highly efficient CO2 splitting at low temperature (<800 °C) due to insufficient activation of metal oxides for CO2. Herein, the introduction of a small amount of Pt was found to be able to greatly increase the performance of CO2 splitting with the highest peak CO production rate of about 65 mL min-1 g-1, CO productivity of about 53 mL g-1, nearly 100 % CO2 conversion and long-term stability for 0.5Pt/CeO2, which exceeded most of the state-of-the-art transition metals-based oxides even at lower temperature (700 °C). This could be attributed to the addition of Pt leading to the formation of an interface (Pt0-Ov-Ce3+) after CH4 reduction, which improved CO2 activation and dissociation due to beneficial breakage of C=O bond by the cooperation of Pt0 and oxygen vacancies in the interface.