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Photocatalytic ethylene production over defective NiO through lattice oxygen participation SCIE
期刊论文 | 2025 , 16 (1) | NATURE COMMUNICATIONS
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Abstract :

Lattice oxygen-mediated photocatalytic ethane dehydrogenation represents a sustainable strategy for ethylene production, yet achieving a balance between high productivity, selectivity, and durability remains challenging. Here, we report a defective NiO-300 catalyst, where precisely engineered Ni vacancies activate lattice oxygen by weakening Ni-O bond and improving lattice oxygen mobility. This promotes efficient ethane activation and C-H bonds cleavage through photoinduced hole capture, intensifying ethane dehydrogenation via a light-boosted Mars-van Krevelen mechanism. The NiO-300 catalyst manifests a high ethylene yield of 604.5 mu mol g-1 h-1 with 100% selectivity and stability over 200 cycles. In situ spectroscopic and theoretical studies elucidate the generation of active oxygen species, the evolution of Ni coordination, the formation of key intermediates, and the underlying photocatalytic mechanism. Our findings highlight cation vacancy engineering as a powerful tactic to fully activate lattice oxygen for solar-driven alkene production from alkane dehydrogenation over oxide photocatalysts.

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GB/T 7714 Wei, Fen , Zhao, Jiwu , Liu, Yu-Chun et al. Photocatalytic ethylene production over defective NiO through lattice oxygen participation [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) .
MLA Wei, Fen et al. "Photocatalytic ethylene production over defective NiO through lattice oxygen participation" . | NATURE COMMUNICATIONS 16 . 1 (2025) .
APA Wei, Fen , Zhao, Jiwu , Liu, Yu-Chun , Hsu, Yung-Hsi , Hung, Sung-Fu , Fu, Junwen et al. Photocatalytic ethylene production over defective NiO through lattice oxygen participation . | NATURE COMMUNICATIONS , 2025 , 16 (1) .
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Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural SCIE
期刊论文 | 2025 | CHEMCATCHEM
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Cyclopentanone (CPO) is a high-value platform chemical widely used in fuel, fragrances, and polymers, yet its sustainable production from biomass remains challenging. This work addresses this gap by developing efficient Ni/TiO2 catalysts through crystal phase engineering of TiO2 supports (anatase, rutile, mixed-phase P25) for aqueous-phase hydrogenative ring-rearrangement of furfural (FAL) to CPO. Crucially, the TiO2 phase dictates the Ni-O-Ti interface structure, governing nickel speciation and reactivity. Ni supported on mixed-phase P25 achieves exceptional performance under industrially relevant conditions: 91.1% FAL conversion, 89.3% CPO selectivity, and specific rate of 71.6 h(-1), surpassing catalysts on pure anatase (9.1% conversion) or rutile (55.8% conversion). Physical mixture experiments confirm this superiority stems from the intrinsic interface of P25, not component blending. Characterization reveals that P25 stabilizes a multifunctional surface ensemble: metallic Ni-0 (18.0% by XPS) enables hydrogenation, while cationic Ni2+ facilitates acid-catalyzed dehydration and ring rearrangement. Simultaneously, sufficient metal-support interaction permits in situ regeneration of active sites. The optimized 1Ni/P25 demonstrates robust stability over five cycles with retained selectivity (>90%), showcasing practical durability. This study provides a scalable design strategy-support crystal phase tuning-to engineer cost-effective, multifunctional catalysts for industrial biomass upgrading, advancing green manufacturing of cyclic ketones without precious metals.

Keyword :

Cyclopentanone Cyclopentanone Furfural Furfural Metal-support interaction Metal-support interaction Ni-O-Ti interface Ni-O-Ti interface TiO2 crystal phase TiO2 crystal phase

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GB/T 7714 Tang, Yu , Xu, Kaiyang , Weng, Lingfeng et al. Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural [J]. | CHEMCATCHEM , 2025 .
MLA Tang, Yu et al. "Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural" . | CHEMCATCHEM (2025) .
APA Tang, Yu , Xu, Kaiyang , Weng, Lingfeng , Xu, Yuanjie , Tan, Li , Wu, Lizhi . Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural . | CHEMCATCHEM , 2025 .
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Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst SCIE
期刊论文 | 2025 , 579 | MOLECULAR CATALYSIS
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Alkali metal promoted Zn/SSZ-13 catalysts were investigated for ethane dehydrogenation (EDH) and CO2assisted oxidative ethane dehydrogenation (CO2-EDH). The Zn/Na/K/SSZ-13 demonstrated enhanced ethane dehydrogenation performance, achieving 0.381 mol C2H4 gZn 0.04 h-1 in the CO2-EDH process after 440 min time on stream, compared to the unmodified Zn/SSZ-13 catalyst. Comprehensive characterizations revealed that the isolated Zn2+ species serve as the active sites for dehydrogenation, while the addition of alkali metals compensate the acid sites of SSZ-13, effectively suppressing the side reactions such as cracking. Moreover, the introduction of CO2 mitigates Zn loss and enhances catalyst activity and stability by coupling with the reverse water gas shift reaction (RWGS), which also suppress the coke deposition. Investigation of vary CO2 content indicated that higher CO2 concentrations significantly suppress Zn loss and increase the proportion of the RWGS reaction, thereby improving CO2-EDH catalytic performance. This work elucidates the active phase of ethane dehydrogenation and highlights the role of alkali metals and CO2 in the CO2-EDH process over Zn/Na/K/SSZ-13, providing valuable insights for designing high-performance CO2EDH catalysts.

Keyword :

Alkaline metal Alkaline metal Carbon dioxide Carbon dioxide Ethane Ethane Ethylene Ethylene Oxidative dehydrogenation Oxidative dehydrogenation Reverse water-gas shift Reverse water-gas shift Zeolite Zeolite Zinc Zinc

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GB/T 7714 Wu, Lizhi , Zheng, Wenchun , Wang, Xiaofang et al. Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst [J]. | MOLECULAR CATALYSIS , 2025 , 579 .
MLA Wu, Lizhi et al. "Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst" . | MOLECULAR CATALYSIS 579 (2025) .
APA Wu, Lizhi , Zheng, Wenchun , Wang, Xiaofang , He, Juncheng , Zou, Caixin , Zhu, Mengjia et al. Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst . | MOLECULAR CATALYSIS , 2025 , 579 .
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Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization SCIE
期刊论文 | 2025 , 71 (5) | AICHE JOURNAL
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Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h-1. According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Pt delta+ species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Br & oslash;nsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.

Keyword :

dehydroaromatization dehydroaromatization Pt/Fe-S-1 Pt/Fe-S-1 the tandem catalysis the tandem catalysis ZSM-5 ZSM-5

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GB/T 7714 Wu, Lizhi , Zhang, Ying , Zou, Caixin et al. Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization [J]. | AICHE JOURNAL , 2025 , 71 (5) .
MLA Wu, Lizhi et al. "Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization" . | AICHE JOURNAL 71 . 5 (2025) .
APA Wu, Lizhi , Zhang, Ying , Zou, Caixin , Sun, Qin , Li, Baozhen , Zheng, Wenchun et al. Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization . | AICHE JOURNAL , 2025 , 71 (5) .
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Insights into morphology-dependent MIL-100(Fe) catalyst towards high efficiency photothermal reduction of CO2 by H2O SCIE
期刊论文 | 2025 , 576 | MOLECULAR CATALYSIS
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The photothermal catalytic CO2 reduction has emerged as a promising technology for the effective use of solar energy and the reduction of greenhouse gas emissions. MIL-100(Fe), as a MOF material, is always considered an excellent catalyst due to its excellent porous structure, low toxicity, extraordinarily high chemical stability and abundant active sites. However, the relationship between morphology and photothermal catalytic CO2 reduction is still being explored and studied. Here, we prepared the MIL-100(Fe) catalysts with different morphologies of nanospheres, nanoparticles and bulk to investigate their photothermal catalytic CO2 reduction performance. The results showed that the nanospherical sample exhibited the highest activity for photothermal CO2 reduction by H2O with CO productivity of 124.04 mu mol center dot g-1 center dot h-1 higher than the other two samples. The characterization results and mechanism analysis indicated that the nanospherical sample had a lower band gap energy value, lower luminescence intensity and stronger transient photocurrent response, which effectively promoted the separation of photo generated electron-hole pairs. More importantly, the AQE calculation results indicated that the nanospherical sample exhibited more lower activation energy in the presence of both light and heat, which is beneficial for photothermal CO2 catalytic to CO. This interesting find will provide experimental evidence for studying the morphology effect on photothermal catalytic CO2 reduction process.

Keyword :

CO2 reduction CO2 reduction MIL-100(Fe) MIL-100(Fe) Morphology Morphology Photothermal catalysis Photothermal catalysis

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GB/T 7714 Wang, Tiaotiao , Zhu, Pengfei , Wang, Maoying et al. Insights into morphology-dependent MIL-100(Fe) catalyst towards high efficiency photothermal reduction of CO2 by H2O [J]. | MOLECULAR CATALYSIS , 2025 , 576 .
MLA Wang, Tiaotiao et al. "Insights into morphology-dependent MIL-100(Fe) catalyst towards high efficiency photothermal reduction of CO2 by H2O" . | MOLECULAR CATALYSIS 576 (2025) .
APA Wang, Tiaotiao , Zhu, Pengfei , Wang, Maoying , Meng, Xinyue , Li, Run , Sun, Longshuai et al. Insights into morphology-dependent MIL-100(Fe) catalyst towards high efficiency photothermal reduction of CO2 by H2O . | MOLECULAR CATALYSIS , 2025 , 576 .
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Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides SCIE
期刊论文 | 2025 , 104 , 66-75 | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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Direct conversion of CO2 into light olefins (C2-C4=) offers a promising approach to mitigating CO2 emissions and lessening reliance on feedstock derived from petroleum-based feedstocks while generating high value-added chemicals. Achieving an effective synergy between Fe3O4 and Fe5C2 is crucial for the hydrogenation of CO2. However, the mechanisms underlying this synergy and strategies for its optimization remain inadequately explored. Herein, we clearly addressed this issue by synthesizing a range of FeNa/NC-x catalysts, wherein the precise control of the Fe5C2/Fe3O4 ratio was manipulated through the adjustment of the initial amount of Fe precursor (denoted by x in the catalysts' names). Among the synthesized catalysts, FeNa/NC-0.6, with the Fe5C2/ Fe3O4 ratio of 2.4, displays the superior CO2 conversion (32.6 %) and STYC2-C4= (54.6 mu molCO2 gFe- 1 s- 1). Moreover, its remarkable C2-C4 = selectivity (47.6 %) and ultra-high STYC2-C4= both fall into a high level among reported Fe-based catalysts for CO2 hydrogenation to light olefins. The excellent catalytic performance can be attributed to the optimized synergistic effect of Fe3O4 and Fe5C2. Reducing the initial amount of Fe precursor weakens the metal-support interaction, which in turn increases the Fe5C2/Fe3O4 ratio. This adjustment results in a perfect balance between the density of CO* intermediates and the quantity of Fe5C2 active sites when the ratio reaches 2.4, thereby enhancing the Fischer-Tropsch synthesis (FTS) process and ultimately improving the catalytic efficiency for CO2 hydrogenation. This paper offers a strategy to optimize synergy of Fe3O4 and Fe5C2 for enhancing catalytic performance and a mechanistic insight, which can be utilized in designing efficient catalysts for other heterogeneous catalytic reactions.

Keyword :

CO 2 hydrogenation CO 2 hydrogenation Iron carbides Iron carbides Iron oxides Iron oxides Light olefins Light olefins Synergistic effect Synergistic effect

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GB/T 7714 Liu, Yunhao , Cheng, Qingpeng , Xiong, Shaohui et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 104 : 66-75 .
MLA Liu, Yunhao et al. "Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 104 (2025) : 66-75 .
APA Liu, Yunhao , Cheng, Qingpeng , Xiong, Shaohui , Zhang, Yingtian , Tan, Li , Song, Song et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 104 , 66-75 .
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Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation SCIE
期刊论文 | 2025 , 505 | CHEMICAL ENGINEERING JOURNAL
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Propane dehydrogenation is one of the most promising routes for propylene production due to its single reactant, product and high economic efficiency. For Co-based catalysts, the state of Co species is one of the important factors affecting the performance of propane dehydrogenation. Here, we designed zeolite Silicalite-1 (S-1) with different silanol nests content as support to investigate the effect of silanol nests content to form Td-Co(II) species. It is found that the content of silanol nests in the S-1 supports have a linear correlation with the formation of Td-Co(II) species and corresponding PDH catalytic activity through the study of the catalyst structure- performance relationship. And the silanol nests of S-1 could be fully coordinated with 0.5 wt% Co content over 0.5Co/S-1-1-HTS in the form of Td-Co(II) species to maximize the Co atomic utilization. Correspondingly, 0.5Co/ S-1-1-HTS shows the most excellent catalytic activity and stability, with C3H6 generation rate of 3014 mmol C 3 H 6 g Co-1 h-1 and deactivation rate of 0.07 h-1 at 550 degrees C.

Keyword :

Hydrothermal treatment Hydrothermal treatment Propane dehydrogenation Propane dehydrogenation Silanol nests Silanol nests Silicalite-1 Silicalite-1 Td-Co(II) Td-Co(II)

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GB/T 7714 Deng, Huihui , Li, Baozhen , Zheng, Wenchun et al. Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 505 .
MLA Deng, Huihui et al. "Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 505 (2025) .
APA Deng, Huihui , Li, Baozhen , Zheng, Wenchun , Sun, Qin , Zhu, Mengjia , Zuo, Jun et al. Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 505 .
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Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst SCIE
期刊论文 | 2025 , 51 (2) , 675-693 | RESEARCH ON CHEMICAL INTERMEDIATES
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The use of bifunctional catalysts, combining methanol synthesis and zeolite components, has been cleverly expanding to the hydrogenation of CO2 into liquefied petroleum gas (LPG). However, such catalysts in this reaction displayed low catalytic efficiency due to the mismatch of the two components. In this study, an efficient strategy was realized via physically coating beta zeolite onto the CuZnAl methanol catalyst, resulting in a shell thickness controllable core-shell encapsulated catalyst, denoted as CuZnAl@beta. Sufficient characterization proves that the micro-coupling structure between methanol active sites and zeolite acid sites is designed reasonably and successfully, as consequently, the zeolite capsule catalysts embody a significant improvement toward LPG selectivity. Hence, the CuZnAl@beta catalyst reached a high selectivity to LPG at 77.9% with 21.3% CO2 conversion, under a reaction pressure of 2.0 MPa and a temperature of 320 degrees C. The strategy employed in this study could offer valuable insights into guiding catalyst design.

Keyword :

beta zeolite beta zeolite Bifunctional active sites Bifunctional active sites Capsule catalyst Capsule catalyst CO2 hydrogenation CO2 hydrogenation Liquefied petroleum gas Liquefied petroleum gas

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GB/T 7714 Zhang, Peipei , Huang, Xin , Qu, Shunli et al. Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst [J]. | RESEARCH ON CHEMICAL INTERMEDIATES , 2025 , 51 (2) : 675-693 .
MLA Zhang, Peipei et al. "Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst" . | RESEARCH ON CHEMICAL INTERMEDIATES 51 . 2 (2025) : 675-693 .
APA Zhang, Peipei , Huang, Xin , Qu, Shunli , Wang, Peng , Mi, Xiaotong , Li, Sixuan et al. Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst . | RESEARCH ON CHEMICAL INTERMEDIATES , 2025 , 51 (2) , 675-693 .
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Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction SCIE
期刊论文 | 2025 , 573 | MOLECULAR CATALYSIS
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The utilization of Cu-based catalysts in the low-temperature catalytic conversion of CO2 to methanol is the focus of industrial processes. However, the metastable nature of highly dispersed Cu active sites causes it easy to sinter, which leads to the decline of activity and methanol selectivity. Herein, an approach involving the incorporation of highly dispersed La species into Cu-ZnO-Al2O3 (CZAL-x) through one-pot synthesis, benefits dispersing and stabilizing Cu0/Cu+ active sites. Consequently, a CO2 conversion reaches 22.4 % with a 75.0 % methanol selectivity of the optimizing CZAL-2.5 catalyst in a stable reaction for 100 h. When the space velocity is 16,000 mL g cat.- 1 h- 1 , the space-time yield of methanol reached the highest value of 814.9 g MeOH kg cat1 h- 1 , significantly outperforming the CZA catalyst. Systematic characterizations reveal the introduction of LaOx enhanced the interaction between Cu active sites and carrier, which effectively improved the sintering resistance of copper nanoparticles.

Keyword :

Anti-sintering Anti-sintering CO2 hydrogenation reaction CO2 hydrogenation reaction Highly dispersed LaOx Highly dispersed LaOx Methanol selectivity Methanol selectivity Robust Cu active sites Robust Cu active sites

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GB/T 7714 Zhang, Peipei , Wang, Wenbo , Wang, Peng et al. Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction [J]. | MOLECULAR CATALYSIS , 2025 , 573 .
MLA Zhang, Peipei et al. "Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction" . | MOLECULAR CATALYSIS 573 (2025) .
APA Zhang, Peipei , Wang, Wenbo , Wang, Peng , Mi, Xiaotong , Xin, Jing , Li, Sixuan et al. Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction . | MOLECULAR CATALYSIS , 2025 , 573 .
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Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol SCIE
期刊论文 | 2025 , 15 (12) , 10068-10081 | ACS CATALYSIS
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The utilization of Rh-based catalysts in the direct production of ethanol from CO2 has been a subject of significant interest. However, to date, the precise active sites responsible for ethanol generation and the C-C coupling mechanism remain elusive. In this study, we present a Rh-based catalyst featuring nanoscale Rh-Fe alloy sites, which achieved an ethanol selectivity of 49.1% among all hydrocarbon and oxygenate products (CO excluded) under relatively mild reaction conditions (3.0 MPa, 200 degrees C, with a low metal loading of <= 1 wt %). The formation of ethanol proceeds via the HCOO* pathway with a CO insertion mechanism occurring at the alloy sites with a specific cluster size, where CH2* and CO* act as the crucial intermediates for C-C coupling. The electron interaction within the Rh-Fe alloy sites effectively reduces the energy barrier for the formation of the CH2CO* intermediate, thereby facilitating the production of ethanol. In contrast to the Rh-Fe alloy sites, the geminal-dicarbonyl binding configuration of CO* intermediates on Rh single sites favors the generation of byproducts such as methane and methanol, rather than ethanol. This research offers insights into the active sites and reaction mechanism of hydrogenation of CO2 to ethanol, thus enhancing the efficient utilization of Rh-based catalysts.

Keyword :

C-C coupling C-C coupling CO2 hydrogenation CO2 hydrogenation ethanol ethanol Rh-Fealloy Rh-Fealloy thermal catalysis thermal catalysis

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GB/T 7714 Chen, Yang , Zhou, Diwen , Chang, Yongli et al. Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol [J]. | ACS CATALYSIS , 2025 , 15 (12) : 10068-10081 .
MLA Chen, Yang et al. "Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol" . | ACS CATALYSIS 15 . 12 (2025) : 10068-10081 .
APA Chen, Yang , Zhou, Diwen , Chang, Yongli , Xu, Yunzhao , Lin, Hongqiao , Wu, Lizhi et al. Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol . | ACS CATALYSIS , 2025 , 15 (12) , 10068-10081 .
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