Freezing copper as a noble metal–like catalyst for preliminary hydrogenation

Sun, Jian; Yu, Jiafeng; Ma, Qingxiang; Meng, Fanqiong; Wei, Xiaoxuan; Sun, Yannan; Tsubaki, Noritatsu

doi:10.1126/sciadv.aau3275

Cited by 76 publications

(68 citation statements)

References 40 publications

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“…For 0.5%-ZnAl-LDH, the Auger signal was broader and less well-defined compared to that collected for CuZnAl-LDH, suggesting the presence of Cu in several valence states in the 0.5%-ZnAl-LDH sample (i.e., Cu + and Cu 2+ ). [27] The XPS and AES results thus provided strong evidence for the presence of electron-rich Cu δ+ in the 0.5%-ZnAl-LDH, which is consistent with the XAS findings.…”

Section: Doi: 101002/aenm201901973supporting

confidence: 81%

“…X‐ray‐excited LMM Auger spectra were also collected for 0.5%‐ZnAl‐LDH and CuZnAl‐LDH to further probe the valence of Cu in these samples (Figure S6d, Supporting Information). For 0.5%‐ZnAl‐LDH, the Auger signal was broader and less well‐defined compared to that collected for CuZnAl‐LDH, suggesting the presence of Cu in several valence states in the 0.5%‐ZnAl‐LDH sample (i.e., Cu + and Cu 2+ ) . The XPS and AES results thus provided strong evidence for the presence of electron‐rich Cu δ + in the 0.5%‐ZnAl‐LDH, which is consistent with the XAS findings.…”

Section: Methodssupporting

confidence: 74%

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Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Zhang

Zhao

Shi

et al. 2020

Advanced Energy Materials

191

114

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The photocatalytic reduction of nitrogen (N2) with water (H2O) as the reducing agent holds great promise as a sustainable future technology for the synthesis of ammonia (NH3). Herein, the effect of oxygen vacancies and electron‐rich Cuδ+ on the performance of zinc‐aluminium layered double hydroxide (ZnAl‐LDH) nanosheet photocatalysts for N2 reduction to NH3 under UV–vis excitation is systematically explored. Results show that a 0.5%‐ZnAl‐LDH nanosheet photocatalyst (containing 0.5 mol% Cu by metal basis) affords a remarkable NH3 production rate of 110 µmol g−1 h−1 and excellent stability in pure water. The X‐ray absorption spectroscopy, electron paramagnetic resonance, and density functional theory calculations reveal that Cu addition imparts oxygen vacancies and coordinatively unsaturated Cuδ+ (δ < 2) with electron‐rich property in the ZnAl‐LDH nanosheets, both of which readily contribute to efficient separation and transfer of photogenerated electrons and holes and promote N2 adsorption, thereby both activating N2 and facilitating its multielectrons reduction to NH3.

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Section: Doi: 101002/aenm201901973supporting

confidence: 81%

Section: Methodssupporting

confidence: 74%

Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Zhang

Zhao

Shi

et al. 2020

Advanced Energy Materials

191

114

View full text Add to dashboard Cite

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“…The different adsorption configuration for acetic acid (Fig. 5g, i, j) has proved that single-atom Ni in Ni-NCNT redistribute the outer electron, affecting the surrounding atom to have a new electronic structure and further alters the material's electronegativity and promote the activity of Ru cluster 17 .the reason of the adsorption for O 2 was less affected by introducing Ni single-atom may be that the new electronic structure was not suitable for O 2 to form Ru-O bond. Therefore, loading noble metal nanoparticle on this transition metal atom anchored support is a facile and reliable strategy for improving the catalytic activity.…”

Section: Resultsmentioning

confidence: 99%

Single-atom nickel confined nanotube superstructure as support for catalytic wet air oxidation of acetic acid

Wei

Sun

et al. 2019

Commun Chem

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Single-atom confined materials (SACMs) have been widely researched as catalysts in many fields within recent years. However, this class of materials may not only serve as a catalyst but also as a support material for certain reactions. Here we propose a general strategy to use SACMs as supports for tuning loaded noble metal (e.g., Ru) nanoparticles with enhanced catalytic activity. As a proof of concept, a nickel single-atom confined nitrogen-doped carbon nanotube (NCNT) superstructure is prepared as a support to load noble metal Ru for catalytic wet air oxidation of acetic acid. Improved catalytic activity with a mineralization rate of 97.5% is achieved. Further, adsorption configurations based on DFT calculations also confirm our deduction that the introduction of single-atom Ni changes the intrinsic property of NCNTs and affects the loaded active Ru nanoparticles.

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“…Over the past few years, non-noble metal catalysts have attracted much attention due to their comparable properties with noble metal catalysts in both homogeneous and heterogeneous catalysis [113][114][115][116][117]. In particular, furfural hydrogenation has been widely tested while using various non-noble metal catalysts, such as Cu, Co, Ni, and Zr, among others.…”

Section: Non-noble Metal Catalystsmentioning

confidence: 99%

Recent Advances in Catalytic Hydrogenation of Furfural

et al. 2019

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Furfural has been considered as one of the most promising platform molecules directly derived from biomass. The hydrogenation of furfural is one of the most versatile reactions to upgrade furanic components to biofuels. For instance, it can lead to plenty of downstream products, such as (tetrahydro)furfuryl alcohol, 2-methyl(tetrahydro)furan, lactones, levulinates, cyclopentanone(l), or diols, etc. The aim of this review is to discuss recent advances in the catalytic hydrogenation of furfural towards (tetrahydro)furfuryl alcohol and 2-methyl(tetrahydro)furan in terms of different non-noble metal and noble metal catalytic systems. Reaction mechanisms that are related to the different catalytic materials and reaction conditions are properly discussed. Selective hydrogenation of furfural could be modified not only by varying the types of catalyst (nature of metal, support, and preparation method) and reaction conditions, but also by altering the reaction regime, namely from batch to continuous flow. In any case, furfural catalytic hydrogenation is an open research line, which represents an attractive option for biomass valorization towards valuable chemicals and fuels.FA is a very important monomer for the synthesis of furan resins, which are widely used in thermoset polymer matrix composites, cements, adhesives, coatings, and casting/foundry resins. This molecule is also used as a non-reactive diluent for epoxy resin, a modifier for phenolic and urea resins, an oil well, and a carbon binder. Furthermore, the salt of FA is used in the synthesis of lysine, vitamin C, lubricants, and plasticizers [22,23]. Moreover, it should be highlighted that FA is also an important intermediate for the production of further hydrogenation products (as shown in Scheme 1), such as 2-methylfuran (MF), a potential alternative fuel with better combustion performance and higher Research Octane Number (RON = 103) than that of gasoline (RON = 96.8) [24]. In other applications, MF is used in perfume intermediates, chloroquine lateral chains in medical intermediates, and as a raw material for the production of chrysanthemate pesticides [25].Moreover, tetrahydrofurfuryl alcohol (THFA) can be used as a green solvent in the pharmaceutical industry and, in addition, it constitutes an outstanding intermediate to produce dihydropyran [26], pyridine [27], tetrahydrofuran, and pentan-1,5-diol [28][29][30]. Particularly, the latest molecule is an important monomer in the plastics industry. Furthermore, 2-methyltetrahydrofuran (MTHF) is quite engaging for its possible applications in organometallic chemistry, as well as in organic reactions that are related to organocatalysis, biotransformations, and biomass processing [31]. Catalysts 2019, 9, 796 3 of 33 Catalysts 2018, 8, x FOR PEER REVIEW 3 of 36 Scheme 1. Illustrative representation of reaction pathways in furfural hydrogenation.Other downstream products of furfural hydrogenation, such as (tetrahydro)furan [32], tetrahydrofurfural [33], lactones [34][35][36][37], levulinates [38,39], cyclopentanone...

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Freezing copper as a noble metal–like catalyst for preliminary hydrogenation

Abstract: Copper is “frozen” into a metallic state as a noble metal–like catalyst for controlling the product in a chemical reaction.

Cited by 76 publications

References 40 publications

Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Single-atom nickel confined nanotube superstructure as support for catalytic wet air oxidation of acetic acid

Recent Advances in Catalytic Hydrogenation of Furfural

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Freezing copper as a noble metal–like catalyst for preliminary hydrogenation

Abstract: Copper is “frozen” into a metallic state as a noble metal–like catalyst for controlling the product in a chemical reaction.

Cited by 76 publications

References 40 publications

Efficient Photocatalytic Nitrogen Fixation over Cuδ+‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Efficient Photocatalytic Nitrogen Fixation over Cuδ+‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Single-atom nickel confined nanotube superstructure as support for catalytic wet air oxidation of acetic acid

Recent Advances in Catalytic Hydrogenation of Furfural

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Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets

Efficient Photocatalytic Nitrogen Fixation over Cu^δ⁺‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets