Fabrication of immobilized nickel nanoclusters decorated by C N  species for cellulose conversion to C2,3 oxygenated compounds: Rational design via typical C- and N-sources

Xiao, Zhuqian; Wang, Xiaolei; Yang, Qifan; Xing, Chuang; Ge, Qing; Gai, Xikun; Mao, Jianwei; Ji, Jianbing

doi:10.1016/j.jechem.2020.02.054

Cited by 6 publications

(7 citation statements)

References 36 publications

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“…The third sample was similar to the second sample with the additional presence of a N-donor molecule, melamine, obtained from urea in order to increase the N content in the carbon support. The presence of hydroxyl and amino groups was expected at the surface of all supports as anchoring sites for depositing metallic species …”

Section: Methodsmentioning

confidence: 99%

“…Such catalyst configuration enhanced EG production, owing to the presence of Ni−N−N Lewis pairs. 28 Recently, Goc et al confirmed the potential of Ni−W x C/AC catalysts for the hydrogenolysis of cellulose into EG and PG. 33 However, property improvement is still awaited, and the quest for supports that stabilize more efficiently the active sites operating under severe hydrothermal conditions is needed.…”

Section: ■ Introductionmentioning

confidence: 98%

“…The retention of the catalyst activity was attributed to the presence of the C 3 N 4 phase and of the Ni–W alloys. Such catalyst configuration enhanced EG production, owing to the presence of Ni–N–N Lewis pairs …”

Section: Introductionmentioning

confidence: 99%

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Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Boulos,

Goc,

Perret

et al. 2024

ACS Appl. Nano Mater.

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Cellulose is an attractive nonedible feedstock for the production of chemicals, especially through metal catalysis. However, its hydrothermal catalytic conversion induces severe deactivation of catalysts, notably by metal leaching and structure sintering. In this work, we studied a series of nickel-and tungstenbased catalysts supported on porous carbon (C) or N-doped porous carbon (NC). These catalysts were formed from nanosized bimetallic particles of Ni and W supported on porous N-doped carbon supports. The supports were prepared by hydrothermal conversion of N-containing biopolymers, followed by pyrolysis under an inert atmosphere. The bimetallic nanoparticles were deposited by wet impregnation. The idea was to study the influence of Ndoping of the support on the stability during the catalysis of the metal nanoparticles on the support. For instance, an amorphous nitrogen-doped carbon with a hierarchical porosity and a surface area up to 286 m 2 •g −1 was obtained from the hydrothermal pyrolysis of chitosan, and, depending on the activation atmosphere (H 2 or N 2 ), metal particles in the 15−30 nm size were obtained. Regarding the application to cellulose conversion, molar yields up to 20% in ethylene glycol and 8% in propylene glycol were obtained by a reaction at 245 °C for 1 h using a nitrogen-activated catalyst. When the catalyst was activated under hydrogen, the ethylene glycol yield was increased to 51% while the propylene glycol yield remained low. Very interestingly, the presence of Ncontaining moieties within the carbon supports proved an interest by increasing the catalyst stability during successive reaction cycles. The ethylene glycol yield remained stable during 3 reaction cycles for the N-doped catalyst, as compared to the nondoped one, which presented an important deactivation after 3 cycles.

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Section: Methodsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 98%

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Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Boulos,

Goc,

Perret

et al. 2024

ACS Appl. Nano Mater.

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“…The C x N y layer and Ni–N structure contributed to the sintering resistance and acid leaching of the Ni–W/SiO 2 @C x N y catalyst. No large scale aggregation was observed with most of the nanoclusters, and the outer C x N y layer could be observed clearly after seven runs . For easier decomposition and reduction of Ni, chelating agents (ammonium hydroxide and ethanediamine) were introduced coupled with an organic reducing agent (EG) to synthesize a SiO 2 -supported Ni–W catalyst without a carbon matrix, where enhanced dispersion could be observed compared with the normal SiO 2 support.…”

Section: C–c Bond Cleavage Transformations Of Carbohydratesmentioning

confidence: 99%

Toward Value-Added Chemicals from Carbohydrates via C–C Bond Cleavage and Coupling Transformations

Zhang,

Liu

et al. 2024

ACS Catal.

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Renewable carbohydrates are nearly inexhaustible libraries of chemical building blocks, and significant research efforts have been devoted to their valorization to valuable chemicals in the past decades. The commonly recognized main transformation routes include dehydration and C−C bond cleavage pathways, which lead to the production of conventional platform chemicals such as 5-hydroxymethylfurfural/furfural, lactic acid/lactates, and so on. With the huge availability of carbohydrates on earth, the production of other fine chemicals is very attractive but remains sparse. This Review therefore emphasizes the utilization strategies of carbohydrates based on in situ C−C bond cleavage to lower carbon fragments, such as glycolaldehyde and erythrose, and their subsequent transformations, e.g. hydrogenation, hydrogenolysis, oxidation, nucleophilic addition, and amination. The isolation of reactive intermediates is avoided, leading to the formation of a variety of "unconventional" useful scaffolds, such as ethylene glycol, ethanol, keto-alcohols, glycolic acid, formic acid, C4 skeleton α-hydroxy esters, N-containing compounds, etc. Inspired by the transformation of active intermediates, the direct conversion of monosugars with similar structures through C−C coupling to furan-based chemicals is also briefly reviewed. The primary focus of this Review is to show the spectacular range of fine chemicals that can be accessed from carbohydrates via C−C bond cleavage and coupling approaches. A summary of the reviewed works and some opportunities and challenges within this attractive field are underlined for future research in sugar chemistry.

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“…[10][11][12] Compared to their counterparts, metal NPs have unique electronic structures, quantum-size effects, rich active surface atoms, and a large surface-to-volume ratio, showing widespread applications in heterogeneous catalysis. [13][14][15][16][17][18][19] Unfortunately, these metal NPs are not uniform at the atomic level, and thus include multiple active sites, showing the property of multiple reaction pathways and low selectivity for most of the catalytic processes. [20,21] The polydispersity of NPs seriously affects the selectivity for desired products and hampers the identification of the active sites and reaction intermediates.…”

Section: Introductionmentioning

confidence: 99%

Programmable kernel structures of atomically precise metal nanoclusters for tailoring catalytic properties

Zhao

Zang

2023

Exploration

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The unclear structures and polydispersity of metal nanoparticles (NPs) seriously hamper the identification of the active sites and the construction of structure‐reactivity relationships. Fortunately, ligand‐protected metal nanoclusters (NCs) with atomically precise structures and monodispersity have become an ideal candidate for understanding the well‐defined correlations between structure and catalytic property at an atomic level. The programmable kernel structures of atomically precise metal NCs provide a fantastic chance to modulate their size, shape, atomic arrangement, and electron state by the precise modulating of the number, type, and location of metal atoms. Thus, the special focus of this review highlights the most recent process in tailoring the catalytic activity and selectivity over metal NCs by precisely controlling their kernel structures. This review is expected to shed light on the in‐depth understanding of metal NCs’ kernel structures and reactivity relationships.

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Fabrication of immobilized nickel nanoclusters decorated by C N species for cellulose conversion to C2,3 oxygenated compounds: Rational design via typical C- and N-sources

Cited by 6 publications

References 36 publications

Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Toward Value-Added Chemicals from Carbohydrates via C–C Bond Cleavage and Coupling Transformations

Programmable kernel structures of atomically precise metal nanoclusters for tailoring catalytic properties

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Fabrication of immobilized nickel nanoclusters decorated by C N species for cellulose conversion to C2,3 oxygenated compounds: Rational design via typical C- and N-sources

Cited by 6 publications

References 36 publications

Cellulose Conversion to Glycols over a Carbon-Supported Ni–WxC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Cellulose Conversion to Glycols over a Carbon-Supported Ni–WxC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Toward Value-Added Chemicals from Carbohydrates via C–C Bond Cleavage and Coupling Transformations

Programmable kernel structures of atomically precise metal nanoclusters for tailoring catalytic properties

Contact Info

Product

Resources

About

Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability

Cellulose Conversion to Glycols over a Carbon-Supported Ni–W_xC Nanocatalyst: The N-Doping Effect on Catalyst Stability