Gallium Switches the Selectivity of Classical Methanation Catalysts to Produce Methanol from CO2 DOI Creative Commons
Wei Zhou, Colin Hansen,

Weicheng Chao

и другие.

Опубликована: Фев. 14, 2024

Carbon dioxide is a major contributor to global climate change and ocean acidification, making efficient capture utilization required step for sustainable development. A pivotal aspect of development close the carbon cycle by converting CO2 with “green” H2 value-added product or fuel, such as methanol. In this context, supported metal catalysts have been extensively investigated, focusing on role promoters and/or supports drive catalytic performance. particular, besides classical like zinc, gallium has emerged an alternative, properties from Cu-based methanol synthesis Ni-, Pd- Pt-based systems. Here, we show that upon addition Ga, selectivity group 8 9 transition-metal elements (Ru, Rh, Os Ir), switched their widely-observed methanation behavior catalysts, highlighting universal propensity Ga in promoting formation. Detailed studies series tailored silica-supported amenable situ spectroscopy, complemented density functional theory (DFT) calculations indicate particularly prone generate stable MGa alloyed nanoparticles, persist during hydrogenation, driving formation while suppressing reaction.

Язык: Английский

Optimizing Pt-Based Alloy Electrocatalysts for Improved Hydrogen Evolution Performance in Alkaline Electrolytes: A Comprehensive Review DOI

Guoliang Gao,

Guang Zhu, Xueli Chen

и другие.

ACS Nano, Год журнала: 2023, Номер 17(21), С. 20804 - 20824

Опубликована: Ноя. 3, 2023

The splitting of water through electrocatalysis offers a sustainable method for the production hydrogen. In alkaline electrolytes, lack protons forces dissociation to occur before hydrogen evolution reaction (HER). While pure Pt is gold standard electrocatalyst in acidic since 5d orbital nearly fully occupied, when it overlaps with molecular water, generates Pauli repulsion. As result, formation Pt–H* bond an environment difficult, which slows HER and negates benefits using catalyst. To overcome this limitation, can be alloyed transition metals, such as Fe, Co, Ni. This approach has potential not only enhance performance but also increase dispersion decrease its usage, thus overall improving catalyst's cost-effectiveness. excellent adsorption ability metals contributes generation proton-rich local near Pt-based alloy that promotes HER. Significant progress been achieved comprehending mechanism manipulation structure composition electrocatalysts based on alloy. objective review analyze condense latest developments It focuses modified alloys clarifies design principles catalytic catalysts from both experimental theoretical perspective. highlights some difficulties encountered during opportunities increasing performance. Finally, guidance development more efficient provided.

Язык: Английский

Процитировано

94
Atomic Cobalt–Silver Dual-Metal Sites Confined on Carbon Nitride with Synergistic Ag Nanoparticles for Enhanced CO2 Photoreduction DOI

Aixin Deng,

En Zhao, Qi Li

и другие.

ACS Nano, Год журнала: 2023, Номер 17(12), С. 11869 - 11881

Опубликована: Июнь 8, 2023

Photocatalytic reduction of CO2 to value-added solar fuels is great significance alleviate the severe environmental and energy crisis. Herein, we report construction a synergistic silver nanoparticle catalyst with adjacent atomic cobalt-silver dual-metal sites on P-doped carbon nitride (Co1Ag(1+n)-PCN) for photocatalytic reduction. The optimized photocatalyst achieves high CO formation rate 46.82 μmol gcat-1 70.1% selectivity in solid-liquid mode without sacrificial agents, which 2.68 2.18-fold compared that exclusive single-atom (Ag1-CN) site (Co1Ag1-PCN) photocatalysts, respectively. closely integrated situ experiments density functional theory calculations unravel electronic metal-support interactions (EMSIs) Ag nanoparticles Ag-N2C2 Co-N6-P promote adsorption CO2* COOH* intermediates form CH4, as well boost enrichment transfer photoexcited electrons. Moreover, atomically dispersed Co-Ag SA serve fast-electron-transfer channel while act electron acceptor enrich separate more photogenerated This work provides general platform delicately design high-performance catalysts highly efficient conversion.

Язык: Английский

Процитировано

64
Nature of metal-support interaction for metal catalysts on oxide supports DOI
Tairan Wang,

Jianyu Hu,

Runhai Ouyang

и другие.

Science, Год журнала: 2024, Номер 386(6724), С. 915 - 920

Опубликована: Ноя. 21, 2024

The metal-support interaction is one of the most important pillars in heterogeneous catalysis, but developing a fundamental theory has been challenging because intricate interfaces. Based on experimental ‎data, interpretable machine learning, theoretical derivation, and first-principles simulations, we established ‎general metal-oxide interactions grounded ‎metal-metal metal-oxygen interactions. applies to metal nanoparticles atoms oxide supports films supports. We found that for late-transition catalysts, metal-metal dominated support effects suboxide encapsulation over nanoparticles. A principle strong occurrence formulated substantiated by extensive ‎experiments including 10 metals 16 ‎oxides. valuable insights revealed (strong) advance interfacial design supported catalysts.

Язык: Английский

Процитировано

45
Constructing Gradient Orbital Coupling to Induce Reactive Metal–Support Interaction in Pt-Carbide Electrocatalysts for Efficient Methanol Oxidation DOI

Shenzhou Li,

Gang Wang,

Houfu Lv

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(26), С. 17659 - 17668

Опубликована: Июнь 21, 2024

Reactive metal-support interaction (RMSI) is an emerging way to regulate the catalytic performance for supported metal catalysts. However, induction of RMSI by thermal reduction often accompanied encapsulation effect on metals, which limits mechanism research and applications RMSI. In this work, a gradient orbital coupling construction strategy was successfully developed induce in Pt-carbide system without reductant, leading formation L1

Язык: Английский

Процитировано

21
Overturning CO2 Hydrogenation Selectivity via Strong Metal–Support Interaction DOI
Wenzhe Zhang,

Heyun Lin,

Wei Yao

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(4), С. 2409 - 2417

Опубликована: Фев. 1, 2024

Strong metal–support interaction (SMSI) is commonly observed for platinum-group metals on reducible oxide supports upon a high-temperature reduction (≥500 °C). Herein, we show that the SMSI state can be constructed over Ru/anatase-TiO2 catalyst using CO2 hydrogenation reaction gas at low temperature of ∼210 °C, which could overturn selectivity from 100% CH4 to >99% CO. It revealed exposed metallic Ru nanoparticles promote formation via formate intermediates temperatures <200 °C. Elevating under H2-containing atmosphere causes evolution active TiOx suboxide form an encapsulated structure Ru@TiOx, changes surface intermediate carboxy species during hydrogenation, thus leading exclusive CO with long-term catalytic stability. The O2-containing treatment Ru@TiOx achieve cyclic switch product between and CH4. This work provides effective strategy modulate very temperature.

Язык: Английский

Процитировано

20
Breaking the Conversion-Selectivity Trade-Off in Methanol Synthesis from CO2 Using Dual Intimate Oxide/Metal Interfaces DOI

Qimeng Sun,

Xinyu Liu,

Qingqing Gu

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(42), С. 28885 - 28894

Опубликована: Сен. 16, 2024

The selective hydrogenation of carbon dioxide (CO

Язык: Английский

Процитировано

13
Recent progress in understanding the nature of active sites for methanol synthesis over Cu/ZnO catalysts DOI
Xinyu Liu, Hengwei Wang, Junling Lu

и другие.

Journal of Catalysis, Год журнала: 2024, Номер 436, С. 115561 - 115561

Опубликована: Май 19, 2024

Язык: Английский

Процитировано

10
Double-Edged Sword Effect of Classical Strong Metal–Support Interaction in Catalysts for CO2 Hydrogenation to CO, Methane, and Methanol DOI
Yu Xie,

Junjie Wen,

Zonglin Li

и другие.

ACS Materials Letters, Год журнала: 2023, Номер 5(10), С. 2629 - 2647

Опубликована: Авг. 30, 2023

Interesting phenomena such as encapsulation, charge transfer, and bond formation, etc. induced by classical strong metal–support interaction (SMSI) during high-temperature reduction have received wide attention for their potential to determine the catalytic behavior of supported metal catalysts. However, a systematically scientific understanding about effects SMSI on CO2 hydrogenation performance is still insufficient primarily due diversities in catalysts reaction conditions. Here, we outline "double-edged sword effects" activity, stability, even selectivity C1 high-value compounds (CO, methane, methanol). Specifically, moderate could efficiently optimize structural electronic properties tune conversion key intermediates involved hydrogenation, thereby enhancing performance. Nevertheless, excessive fatal methanation methanol synthesis catalysts, because encapsulation active centers suppresses further reactive intermediates. Additionally, alter regulating dissociation H2 breakage C–O bonds. Subsequently, dependencies are emphasized with aim providing guidance developing an appropriate rational design. To conclude, highlighted perspectives deeper also presented.

Язык: Английский

Процитировано

22
Insight into the Dynamic Evolution of Supported Metal Catalysts by In Situ/Operando Techniques and Theoretical Simulations DOI
Yao Nian, Xinyuan Huang, Menghui Liu

и другие.

ACS Catalysis, Год журнала: 2023, Номер 13(16), С. 11164 - 11171

Опубликована: Авг. 8, 2023

ADVERTISEMENT RETURN TO ISSUEPREVViewpointNEXTInsight into the Dynamic Evolution of Supported Metal Catalysts by In Situ/Operando Techniques and Theoretical SimulationsYao NianYao NianSchool Chemical Engineering Technology, Tianjin University, 300072, ChinaHaihe Laboratory Sustainable Transformations, 300192, ChinaMore Yao Nianhttps://orcid.org/0000-0001-7999-7437, Xinyuan HuangXinyuan HuangSchool Huang, Menghui LiuMenghui LiuSchool Liu, Jinli ZhangJinli ZhangSchool Zhanghttps://orcid.org/0000-0001-5805-3824, You Han*You HanSchool China*Email: [email protected]More Hanhttps://orcid.org/0000-0002-6903-0844Cite this: ACS Catal. 2023, 13, 16, 11164–11171Publication Date (Web):August 8, 2023Publication History Received25 May 2023Published online8 August inissue 18 2023https://pubs.acs.org/doi/10.1021/acscatal.3c02370https://doi.org/10.1021/acscatal.3c02370article-commentaryACS PublicationsCopyright © 2023 American Society. This publication is available under these Terms Use. Request reuse permissions free to access through this site. Learn MoreArticle Views2507Altmetric-Citations2LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence for given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail (4 MB) Get e-AlertscloseSUBJECTS:Catalysts,Evolution reactions,Gold,Metal clusters,Metals e-Alerts

Язык: Английский

Процитировано

18
The Role of Mo Single Atoms and Clusters in Enhancing Pt Catalyst for Benzene Hydrogenation: Distinguishing Between Benzene Spillover and Electronic Effect DOI
Zhuo Li,

Fanchun Meng,

Xinchun Yang

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(7), С. 5016 - 5026

Опубликована: Март 19, 2024

Reactant spillover and electronic effects are two indistinguishable factors that influence MoO3 promoters in benzene hydrogenation on Pt-MoO3 catalysts. Previous studies have primarily focused the significance of hydrogen while neglecting transfer effect originating from MoO3. Herein, we synthesized Pt/CNT, Pt–Mo1/CNT with Mo single atoms, Pt–Mocluster/CNT MoOx cluster by using atomic layer deposition. The catalyst exhibited higher activity (3361.8 h–1) at 50 °C, which was twice as high Pt/CNT. In contrast, presence closely interacting clusters Pt nanoparticles inhibited catalyst. Kinetic experiments, DFT calculations, situ FTIR, AIMD simulations revealed atoms multiwalled carbon nanotubes did not alter structure or state but enhanced their increasing coverage via spillover. On other hand, although increased promoters, changes resulted a energy barrier for rate-determining step.

Язык: Английский

Процитировано

9