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Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH SCIE
期刊论文 | 2025 | ADVANCED FUNCTIONAL MATERIALS
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Abstract :

CH3OH is the most desired product of photocatalytic CH4 conversion. The prominent metal-decorated photocatalyst is challenging in both high yield and selectivity for CH3OH products due to over-oxidation by center dot OH mechanism. Here, interstitial Zn is fabricated into ZniO to induce the formation of Zn atom island for rapid single electron reduction of O2 into center dot OOH instead of center dot OH for the selective combination with methyl into CH3OOH. AuPd alloy is simultaneously decorated on ZniO surface for tuning CH3OOH adsorption and reduction into CH3OH. The synergy of Zn atom island and AuPd alloy achieve a tandem reaction pathway (CH4 -> CH3OOH -> CH3OH) for an unprecedented CH3OH yield of 2444 mmol gAuPd-1 h-1 (or 8800 mu mol gcat-1 h-1) with 98.3% selectivity, which bypasses the center dot OH mechanism for tuning the high selectivity of CH3OH. An apparent quantum efficiency of 18.53% at 370 nm for CH4 conversion are super to the reported photocatalytic systems. Thus, this work provides the new strategy of the synergetic atom island and metal alloy photocatalysts through a tandem reaction pathway to mediate the photocatalytic selective oxidation of CH4 into the desired CH3OH.

Keyword :

atom island atom island AuPd alloy AuPd alloy methanol selectivity methanol selectivity photocatalysis photocatalysis tandem reaction tandem reaction

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GB/T 7714 Xiao, Zhen , Shen, Jinni , Jiang, Jianing et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 .
MLA Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS (2025) .
APA Xiao, Zhen , Shen, Jinni , Jiang, Jianing , Zhang, Jiangjie , Liang, Shuqi , Han, Shitong et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH . | ADVANCED FUNCTIONAL MATERIALS , 2025 .
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Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH Scopus
期刊论文 | 2025 | Advanced Functional Materials
Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles SCIE
期刊论文 | 2025 , 361 | SEPARATION AND PURIFICATION TECHNOLOGY
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Abstract :

Localized surface plasmon resonance (LSPR) on base-metal nanoparticles holds significant potential for applications in diverse fields owing to its capability for electric field enhancement. Nevertheless, the efficiency of single-energy conversion remains a limiting factor for LSPR applications. This study investigated the utilization of hot carriers, generated through the LSPR effect in copper nanoparticles (Cu NPs) supported on ZrO2, to enhance the performance of the thermal catalytic reverse water-gas shift (RWGS) reaction. Finite difference time domain simulations and Kelvin probe force microscopy (KPFM) tests demonstrated that LSPR induces a strong electric field, facilitating the excitation of hot carriers in Cu NPs. In-situ DRIFTS analysis revealed that hot electrons promote the formation of formate species (HCOO*) and their subsequent transformation into CO, identified as the rate-determining step. Furthermore, in-situ H2 pulse and quasi-in situ EPR analyses indicated that photo-assisted thermal conditions enhance the conversion of H2 into active hydrogen species (H* or H + ) on Cu NPs, promoting the generation of oxygen vacancies and the transformation of intermediates. Constrained density functional theory calculations further demonstrated that visible light irradiation reduces energy barriers, thereby increasing reaction efficiency. The findings provide valuable insights into the contribution of LSPR-induced hot electrons in advancing the RWGS reaction.

Keyword :

Cu/ZrO 2 Cu/ZrO 2 Hot carriers Hot carriers Localized surface plasmon resonance Localized surface plasmon resonance Oxygen vacancies Oxygen vacancies Reverse water gas shift reaction Reverse water gas shift reaction

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GB/T 7714 Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 .
MLA Ni, Wenkang et al. "Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles" . | SEPARATION AND PURIFICATION TECHNOLOGY 361 (2025) .
APA Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu , Zhang, Zizhong , Zhang, Yongfan , Wang, Ke et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 .
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Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles Scopus
期刊论文 | 2025 , 361 | Separation and Purification Technology
Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles EI
期刊论文 | 2025 , 361 | Separation and Purification Technology
Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder SCIE
期刊论文 | 2025 , 64 (9) | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
WoS CC Cited Count: 1
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Abstract :

H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost-effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three-component photocatalyst, Co(5 %)-HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O2 and H2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.

Keyword :

carbon nitride chips carbon nitride chips overall water splitting overall water splitting photocatalytic photocatalytic PPOWS decoupling PPOWS decoupling reaction mechanism reaction mechanism

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GB/T 7714 Liu, Dan , Xu, Huihui , Shen, Jinni et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) .
MLA Liu, Dan et al. "Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) .
APA Liu, Dan , Xu, Huihui , Shen, Jinni , Wang, Xun , Qiu, Chengwei , Lin, Huaxiang et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) .
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Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder Scopus
期刊论文 | 2025 , 64 (9) | Angewandte Chemie - International Edition
Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder EI
期刊论文 | 2025 , 64 (9) | Angewandte Chemie - International Edition
Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation Scopus
期刊论文 | 2024 , 710 | Journal of Membrane Science
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Abstract :

Membrane distillation technology, utilized for treating hypersaline wastewater from seawater desalination, often encounters challenges related to inorganic scaling, adversely affecting membrane performance. Herein, we introduce a innovative approach employing a sacrificial layer on the surface of Thin Film Composite (TFC) membranes to concurrently enhance inorganic scaling resistance and facilitate membrane reusability. The sacrificial layer (Fe3+-TA) consisted of tannic acid (TA) complexed with iron ions (Fe3+) and could be removed and regenerated in situ. The results demonstrated that the Fe3+-TA layer significantly improved the membrane's surface smoothness and densification, maintaining superior anti-scaling performance. The modified membrane exhibited remarkable durability, sustaining six reuse cycles with a flux recovery exceeding 97 % in gypsum scaling tests. Furthermore, the formation of new complexes during gypsum scaling tests confirmed the membrane's augmented scaling retardation capabilities. Thus, integrating of a sacrificial layer into TFC membranes presents a promising strategy for advancing membrane distillation processes in hypersaline wastewater treatment. © 2024 Elsevier B.V.

Keyword :

Anti-scaling Anti-scaling Inorganic scaling Inorganic scaling Membrane distillation Membrane distillation Reuse Reuse Sacrificial protective layer Sacrificial protective layer

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GB/T 7714 Yan, Z. , Lin, S. , Chang, H. et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation [J]. | Journal of Membrane Science , 2024 , 710 .
MLA Yan, Z. et al. "Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation" . | Journal of Membrane Science 710 (2024) .
APA Yan, Z. , Lin, S. , Chang, H. , Xu, J. , Dai, W. , Qu, D. et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation . | Journal of Membrane Science , 2024 , 710 .
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Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction Scopus
期刊论文 | 2024 , 674 , 158-167 | Journal of Colloid and Interface Science
SCOPUS Cited Count: 6
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Abstract :

Constructing strong interfacial electric fields to enhance the surface charge transport kinetics is an effective strategy for promoting CO2 conversion. Herein, we present the fabrication of CdS-Bi2MoO6 Z-scheme heterojunctions with a robust internal electric field (IEF) using an in situ growth technique, establishing chemical bonding between the components. The IEF at the interface can offer an impetus for the segregation and transportation of photogenerated carriers, while the Cd-O chemical bonding mode acts as a rapid conduit for these carriers, thereby reducing the charge transfer distance. As a result, the Z-scheme charge transfer is accelerated due to the synergistic influence of these two factors. Therefore, the optimized CdS/Bi2MoO6 Z-scheme heterojunction possesses significantly enhanced dynamic carrier mobility, thus promoting the conversion of CO2 to CO without the need for additional co-catalysts or sacrificial agents. This optimization yields a remarkable CO selectivity of up to 97%. Meanwhile, the expedited Z-scheme charge transfer mechanism is validated through X-ray photoelectron spectroscopy, Kelvin probe force microscopy, and in situ diffuse reflectance infrared Fourier transform spectroscopy. © 2024 Elsevier Inc.

Keyword :

Chemical bond Chemical bond CO2 reduction CO2 reduction Internal electric field Internal electric field Photocatalysis Photocatalysis Z-scheme Z-scheme

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GB/T 7714 Wu, Y. , Xiao, J. , Yuan, J. et al. Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction [J]. | Journal of Colloid and Interface Science , 2024 , 674 : 158-167 .
MLA Wu, Y. et al. "Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction" . | Journal of Colloid and Interface Science 674 (2024) : 158-167 .
APA Wu, Y. , Xiao, J. , Yuan, J. , Wang, L. , Luo, S. , Zhang, Z. et al. Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction . | Journal of Colloid and Interface Science , 2024 , 674 , 158-167 .
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Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect SCIE
期刊论文 | 2024 , 197 , 32-45 | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
WoS CC Cited Count: 3
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Abstract :

Optimizing the local surface plasmon resonance (LSPR) effect of non-noble metals through alloying has been crucial for improving its practical application in the field of photocatalysis. Rare studies capture the detail that the change in the electronic structure of metal elements caused by alloying affects plasma carrier concentration and the local surface plasmon resonance effect. Herein, NiCuCoFe medium-entropy alloys (MEAs) nanoclusters were designed and used to modify the Bi3 O4 Br/CNNs Z-scheme heterojunction. The cocktail effect of MEAs causes the 3d-orbital hybridization of various metal elements, which promotes the release of charge carriers. The higher the carrier concentration, the stronger the LSPR effect of MEAs. In addition, the mechanism of three typical working pathways of the LSPR effect to improve the photocatalytic performance of heterojunction is discussed. And compared with those of Bi3 O4 Br, CNNs, and Bi3 O4 Br/CNNs, the rate constant of MEAs-Bi3 O4 Br/CNNs was 3.26, 11.16, and 3.17 times higher during the degradation of norfloxacin, respectively. This study provides a new strategy for understanding the mechanism of LSPR and the rational design of plasmonic coupling architectures for enhanced photocatalysis. (c) 2024 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Keyword :

LSPR LSPR NiCuCoFe medium-entropy alloys NiCuCoFe medium-entropy alloys Orbital hybridization Orbital hybridization Photocatalysis Photocatalysis Z-scheme heterojunction Z-scheme heterojunction

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GB/T 7714 Li, Jianfei , Zhang, Nuotong , Li, Degang et al. Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect [J]. | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 197 : 32-45 .
MLA Li, Jianfei et al. "Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect" . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY 197 (2024) : 32-45 .
APA Li, Jianfei , Zhang, Nuotong , Li, Degang , Li, Yueyun , Zhang, Weimin , Zhao, Zengdian et al. Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 197 , 32-45 .
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Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect EI CSCD
期刊论文 | 2024 , 197 , 32-45 | Journal of Materials Science and Technology
Construction of medium-entropy alloys coupled Z-Scheme heterojunction and its enhanced photocatalytic performance by regulating mechanism of LSPR effect Scopus CSCD
期刊论文 | 2024 , 197 , 32-45 | Journal of Materials Science and Technology
Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O SCIE
期刊论文 | 2024 , 18 (15) , 10582-10595 | ACS NANO
WoS CC Cited Count: 1
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Abstract :

CO2 conversion with pure H2O into CH3OH and O-2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH3OH is significantly challenging. Here we report an organozinc complex/MoS2 heterostructure linked by well-defined zinc-sulfur covalent bonds derived by the structural deformation and intensive coupling of dx 2 - y2(Zn)-p(S) orbitals at the interface, resulting in distinctive charge transfer behaviors and excellent redox capabilities as revealed by experimental characterizations and firstprinciple calculations. The synthesis strategy is further generalized to more organometallic compounds, achieving various heterostructures for CO2 photoreduction. The optimal catalyst delivers a promising CH3OH yield of 2.57 mmol gcat-1 h(-1) and selectivity of more than 99.5%. The reverse water gas shift mechanism is identified for methanol formation. Meanwhile, energy-unfavorable adsorption of methanol on MoS2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.

Keyword :

CO2 photoreduction CO2 photoreduction extraterrestrial synthesis extraterrestrial synthesis methanol methanol strong metal-supportinteractions strong metal-supportinteractions two-dimensional heterostructures two-dimensional heterostructures

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GB/T 7714 Cheng, Ming , Cao, Ning , Wang, Zhi et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O [J]. | ACS NANO , 2024 , 18 (15) : 10582-10595 .
MLA Cheng, Ming et al. "Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O" . | ACS NANO 18 . 15 (2024) : 10582-10595 .
APA Cheng, Ming , Cao, Ning , Wang, Zhi , Wang, Ke , Pu, Tiancheng , Li, Yukun et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O . | ACS NANO , 2024 , 18 (15) , 10582-10595 .
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Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O EI
期刊论文 | 2024 , 18 (15) , 10582-10595 | ACS Nano
Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O Scopus
期刊论文 | 2024 , 18 (15) , 10582-10595 | ACS Nano
Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation SCIE
期刊论文 | 2024 , 710 | JOURNAL OF MEMBRANE SCIENCE
WoS CC Cited Count: 4
Abstract&Keyword Cite Version(2)

Abstract :

Membrane distillation technology, utilized for treating hypersaline wastewater from seawater desalination, often encounters challenges related to inorganic scaling, adversely affecting membrane performance. Herein, we introduce a innovative approach employing a sacrificial layer on the surface of Thin Film Composite (TFC) membranes to concurrently enhance inorganic scaling resistance and facilitate membrane reusability. The sacrificial layer (Fe3+-TA) 3 +-TA) consisted of tannic acid (TA) complexed with iron ions (Fe3+) 3 + ) and could be removed and regenerated in situ. The results demonstrated that the Fe3+-TA 3 +-TA layer significantly improved the membrane's surface smoothness and densification, maintaining superior anti-scaling performance. The modified membrane exhibited remarkable durability, sustaining six reuse cycles with a flux recovery exceeding 97 % in gypsum scaling tests. Furthermore, the formation of new complexes during gypsum scaling tests confirmed the membrane's augmented scaling retardation capabilities. Thus, integrating of a sacrificial layer into TFC membranes presents a promising strategy for advancing membrane distillation processes in hypersaline wastewater treatment.

Keyword :

Anti-scaling Anti-scaling Inorganic scaling Inorganic scaling Membrane distillation Membrane distillation Reuse Reuse Sacrificial protective layer Sacrificial protective layer

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GB/T 7714 Yan, Zhongsen , Lin, Sufen , Chang, Haiqing et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation [J]. | JOURNAL OF MEMBRANE SCIENCE , 2024 , 710 .
MLA Yan, Zhongsen et al. "Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation" . | JOURNAL OF MEMBRANE SCIENCE 710 (2024) .
APA Yan, Zhongsen , Lin, Sufen , Chang, Haiqing , Xu, Junge , Dai, Wenxin , Qu, Dan et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation . | JOURNAL OF MEMBRANE SCIENCE , 2024 , 710 .
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Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation Scopus
期刊论文 | 2024 , 710 | Journal of Membrane Science
Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation EI
期刊论文 | 2024 , 710 | Journal of Membrane Science
Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies SCIE
期刊论文 | 2024 , 492 | CHEMICAL ENGINEERING JOURNAL
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Abstract :

The progressive transfer of photogenerated electrons between the catalyst components and reactants is of great significance for photocatalysis. Amorphous Pd (PdA) and oxygen vacancies (VOs) were simultaneously introduced in Pd-In2O3 exploiting hydrogen-induced amorphization effects; 0.6 wt% Pd-In2O3 exhibited a 4.5-fold increase in activity and a 3.2-fold higher selectivity toward CH3OH + CO (63.62 %) compared with In2O3. Multiple in situ techniques and theoretical calculations revealed that intercomponent electron transfer channels were established via various interface structures formed between PdA or crystalline Pd (PdC) and In2O3; PdA acted as electronic pump, facilitating the transfer and separation of photogenerated electrons, resulting in their subsequent enrichment on the surface of PdA. Simultaneously, PdA acted as electron-donating adsorption site for H2O, increasing the number of electrons received by H2O, further inhibiting the competitive adsorption of H2O and CO2 on VO sites, and promoting the hydrogen evolution reaction. Additionally, the electronic coupling between PdC and VOs could significantly decrease the electron-donating ability of VOs, reducing the number of electrons received by CO2, thus effectively regulating the degree of CO2 reduction. This study employs PdA/PdC and VOs to synergistic optimize the progressive transfer of photogenerated electrons, and presents a novel approach for elucidating the catalytic mechanism.

Keyword :

Adsorption Behavior Adsorption Behavior Amorphous Pd Amorphous Pd CO 2 Photoreduction CO 2 Photoreduction Electron Transfer Electron Transfer Oxygen Vacancies Oxygen Vacancies

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GB/T 7714 Wang, Zhongming , Yuan, Hang , Chen, Siting et al. Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 .
MLA Wang, Zhongming et al. "Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies" . | CHEMICAL ENGINEERING JOURNAL 492 (2024) .
APA Wang, Zhongming , Yuan, Hang , Chen, Siting , Jia, Yong , Guo, Lina , Wang, Hong et al. Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies . | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 .
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Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies EI
期刊论文 | 2024 , 492 | Chemical Engineering Journal
Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies Scopus
期刊论文 | 2024 , 492 | Chemical Engineering Journal
Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies SCIE
期刊论文 | 2024 , 350 | SEPARATION AND PURIFICATION TECHNOLOGY
WoS CC Cited Count: 9
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Abstract :

CO2 is a viable renewable energy source, as global CO2 emissions are perennially increasing. The decomposition of CO2 to CO and O2 through high-temperature cracking of metal oxides via a two-step thermochemical cycle has been an effective strategy to reduce CO2 concentrations in the atmosphere. However, this thermochemical cycle requires a high reaction temperature (1273 K). Hence, in this study, we investigated photothermal CO2 decomposition over three CeO2 catalysts with different morphologies: porous CeO2 nanosheets (2D-CeO2), cubicshaped CeO2 (C-CeO2), and octahedral CeO2 (O-CeO2). The photothermal synergistic effect eliminated the necessity of high temperatures, where light illumination increased the generation of oxygen vacancies and electron transfer to promote CO2 decomposition. The maximum rate of CO production by 2D-CeO2 at 250 degrees C was 69 mu mol g-1h-1, which is significantly higher than those of O-CeO2 (47 mu mol g-1h- 1) and C-CeO2 (19 mu mol g-1h- 1). However, no activity was observed in dark conditions, even at 250 degrees C. In-situ DRIFTS, quasi in-situ EPR, XPS, and Ar-TPD experiments revealed that light irradiation promotes the production of oxygen vacancies on the catalyst surface and generates the intermediate CO2 center dot- species, which cleave the C=O bonds and CO2 conversion, while temperature promotes the adsorption of CO2 on the catalyst surface and facilitates electron transfer. DFT calculations revealed the differences in oxygen vacancy formation and CO2 adsorption among various exposed crystal facets of CeO2. These findings provide new avenues for CO2 decomposition based on the adsorption and activation of CO2 on metal oxide surfaces and the low-temperature synergistic photothermal effect.

Keyword :

CeO2 CeO2 CO2 decomposition CO2 decomposition Oxygen vacancies Oxygen vacancies Photothermal catalysis Photothermal catalysis

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GB/T 7714 Zheng, Duojia , Yue, Xuanyu , Wang, Zhijie et al. Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 350 .
MLA Zheng, Duojia et al. "Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies" . | SEPARATION AND PURIFICATION TECHNOLOGY 350 (2024) .
APA Zheng, Duojia , Yue, Xuanyu , Wang, Zhijie , Fan, Shipeng , Zhang, Zizhong , Dai, Wenxin et al. Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 350 .
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Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies Scopus
期刊论文 | 2024 , 350 | Separation and Purification Technology
Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies EI
期刊论文 | 2024 , 350 | Separation and Purification Technology
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