Three-dimensional flower-like nickel phyllosilicates for CO<sub>2</sub>methanation: enhanced catalytic activity and high stability

Zhang, Tengfei; Tian, Zhiwei; Liu, Qing

doi:10.1039/d0se00360c

Cited by 19 publications

(9 citation statements)

References 47 publications

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“…The Ni crystal size of N/D-100-12, N/D-120-6, N/D-120-12, N/D-120-18, and N/D-140-12 is 4.6, 4.6, 4.7, 5.0, and 5.2 nm (Table 1), respectively, which can retain small Ni particles after high-temperature reduction derived from the strong metal−support interaction of Ni-phyllosilicates. 11,12 Furthermore, for the N/D-120-12-H sample prepared by the conventional hydrothermal method at 120 °C for 12 h, there is only a wide peak attributed to amorphous silica, indicating that no Ni-phyllosilicate is formed under such mild hydrothermal conditions without assistance of NH 4 F and urea (Figure S1). When the severe hydrothermal condition of 220 °C for 48 h is used, the N/D-220-48-H sample displays the typical diffraction peaks belonging to Ni-phyllosilicate (Ni 3 Si 2 O 5 (OH) 4 ) (Figure S2A), suggesting that the Ni-phyllosilicate can be formed using the conventional hydrothermal method through the reaction of biomass-based silica and nickel nitrate under severe hydrothermal conditions.…”

Section: X-ray Diffraction Analysismentioning

confidence: 99%

“…However, there are still some shortcomings for these methods, such as the complicated process, high cost, difficult large-scale production, loss of activity due to partial embedding of Ni particles or poor mass transfer, and so forth . It is reported that the Ni/SiO 2 catalyst can be achieved after the reduction of nickel phyllosilicates, which offers strong interaction between nickel and silica with fine Ni particles at high Ni content and exhibits high catalytic activity without the agglomeration of Ni particles. , Thus, construction and regulation of Ni-phyllosilicates are a promising solution to obtain a high Ni anti-sintering property for the Ni/SiO 2 catalyst.…”

Section: Introductionmentioning

confidence: 99%

“…7 It is reported that the Ni/SiO 2 catalyst can be achieved after the reduction of nickel phyllosilicates, which offers strong interaction between nickel and silica with fine Ni particles at high Ni content and exhibits high catalytic activity without the agglomeration of Ni particles. 11,12 Thus, construction and regulation of Ni-phyllosilicates are a promising solution to obtain a high Ni anti-sintering property for the Ni/SiO 13−15 Ni-phyllosilicates with different crystal structures are usually synthesized by ammonia evaporation or a hydrothermal method through the interaction between Ni precursors and silica-based materials. The ammonia evaporation method refers to the addition of an alkaline reagent (ammonia solution, 16,17 ammonia monohydrate, 18 ammonium chloride, 14 etc.)…”

Section: Introductionmentioning

confidence: 99%

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Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Chen

Liu

2021

ACS Catal.

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Nickel phyllosilicate materials were usually prepared by the conventional hydrothermal method under severe conditions and ammonia evaporation method with unavoidable ammonia emission. To address these problems, a versatile double-accelerator method was proposed in this work, which could successfully synthesize nickel phyllosilicates through the hydrothermal treatment of silica and nickel nitrate at a quite low temperature of 40 °C or in an open system at 80 °C without autogenous pressure assisted by ammonium fluoride (NH4F) and urea. NH4F could accelerate the etching of silica to form the intermediate H4SiO4, and urea could facilitate the formation of a Ni(OH)2 intermediate, resulting in the quick formation of Ni-phyllosilicates. In addition, this method exhibited high universality to prepare various metal (Ni, Co, and Cu) phyllosilicates, and both silica materials and sodium metasilicate could be the potential silicon-containing precursors to prepare Ni-phyllosilicates. Furthermore, the sintered Ni/SiO2 catalyst could also be regenerated after in situ acid pickling and double-accelerator synthesis without decline of catalytic activity. The optimal Ni-phyllosilicate catalyst (N/D-120-12) prepared by the double-accelerator method exhibited a high CO2 conversion of 78.4% and a CH4 yield of 74.5% at 400 °C, which also obtained a low E a of 63.93 kJ·mol–1 and a high TOFCO2 (160 °C) of 3.1 × 10–2 s–1 for CO2 methanation. In situ DRIFTS results demonstrated that the presence of more m-HCOO– species on N/D-120-12 resulted in its high catalytic performance. Moreover, N/D-120-12 also exhibited high long-term and hydrothermal stability with an excellent anti-sintering property.

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Section: X-ray Diffraction Analysismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Chen

Liu

2021

ACS Catal.

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“…For the Ni/SiO 2 -AE catalyst synthesized by the ammonia evaporation method, no phase of nickel oxide was observed, but only the phase of nickel phyllosilicate was shown, and 34.1, 36.7, and 60.5 were characteristic diffraction peaks of nickel silicate, Ni 3 Si 2 O 9 H 4 (JCPDS no. 49-1859) ( Zhang T et al, 2020 ; Chen et al, 2021 ; Zhang and Liu, 2021 ). Meanwhile, the distribution of nickel species was relatively uniform.…”

Section: Resultsmentioning

confidence: 99%

Impact of preparation method on nickel speciation and methane dry reforming performance of Ni/SiO2 catalysts

et al. 2022

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The methane dry reforming reaction can simultaneously convert two greenhouse gases (CH4 and CO2), which has significantly environmental and economic benefits. Nickel-based catalysts have been widely used in methane dry reforming in past decade due to their low cost and high activity. However, the sintering and coke deposition of catalysts severely limit their industrial applications. In this paper, three Ni/SiO2 catalysts prepared by different methods were systematically studied, and the samples obtained by the ammonia evaporation method exhibited excellent catalytic performance. The characterization results such as H2-TPR, XPS and TEM confirmed that the excellent performance was mainly attributed to the catalyst with smaller Ni particles, stronger metal-support interactions, and abundant Ni-O-Si units on the catalyst surface. The anti-sintering/-coking properties of the catalyst were significantly improved. However, the Ni/SiO2-IM catalyst prepared by impregnation method had uneven distribution of nickel species and large particles, and weak metal-support interactions, showing poor catalytic performance in methane dry reforming. Since the nickel species were encapsulated by the SiO4 tetrahedral network, the Ni/SiO2-SG catalyst prepared by sol-gel method could not expose more effective active sites even if the nickel species were uniformly dispersed, resulting in poor dry reforming performance. This study provides guidance for the preparation of novel anti-sintering/-coking nickel-based catalysts.

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“…As we know, "nanosheet" is the typical morphology of phyllosilicates, and the SEM results provide the intuitive evidence of the successful formation of phyllosilicates. 32,33 thermal reaction process, SR can serve as the silica sacrificial template and react with the nickel salt to convert to nickel phyllosilicate with the increase of temperature (Figure 1h). Moreover, the prepared Ni-phyllosilicate catalysts exhibit high mechanical stability, which can retain the nanosheet-like morphology after ultrasonication for 20 min.…”

Section: Resultsmentioning

confidence: 99%

Highly Efficient Ni-Phyllosilicate Catalyst with Surface and Interface Confinement for CO₂ and CO Methanation

Yang

Liu

2021

Ind. Eng. Chem. Res.

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For the conventional Ni/SiO 2 catalyst, it is a challenge to address the sintering problem of Ni particles, especially at high Ni loading. A series of Ni-phyllosilicate catalysts were prepared through the hydrothermal reaction of mesoporous SiO 2 nanorods (SRs) and nickel nitrate, followed by an impregnation modification of CeO 2 . Hydrothermal temperature played an important role in the formation of nickel phyllosilicate. A small amount of Ni-phyllosilicate with a Ni content of 18.56 or 23.88 wt % was formed at a low hydrothermal temperature of 120 or 160 °C, and a large amount of nanosheet-like Ni-phyllosilicate with the Ni content as high as 31.65 wt % was obtained at a high hydrothermal temperature of 200 °C. The prepared Niphyllosilicate catalysts were beneficial to obtain Ni particles with small sizes (3.3−6.3 nm), even though they were reduced at 750 °C and possessed high Ni loadings (18.56−31.65 wt %) owing to the surface and interface confinement of nickel phyllosilicate. After the modification of CeO 2 using an impregnation method, the CeO 2 promoter could further reduce the Ni particle size and increase hydrogen and carbon dioxide uptakes. The CeO 2 -modified Niphyllosilicate catalyst (NPS-180-5C) was the best catalyst in this work, which could reach the thermodynamic equilibrium of CO methanation above 350 °C and exhibited high catalytic activity for CO 2 methanation. In addition, for the 55 °C-100 h-lifetime test for CO 2 methanation and 600 °C-6 h-100% steam treatment tests, NPS-180-5C also showed an excellent antisintering property and higher hydrothermal stability than the impregnated one (N/SR-Im) owing to its special structure and confinement effect as well as promotion of CeO 2 species. In all, the CeO 2 -modified SR-derived Ni-phyllosilicate catalyst could not only effectively suppress the problem of easy sintering of metallic Ni particles on the conventional Ni/SiO 2 catalysts but also exhibit high catalytic activity and hydrothermal stability, which was a promising catalyst for both CO 2 and CO methanation reactions.

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Three-dimensional flower-like nickel phyllosilicates for CO₂methanation: enhanced catalytic activity and high stability

Abstract: A group of MCF-derived nickel phyllosilicates were designed and synthesized by a hydrothermal method for enhanced CO2 methanation.

Cited by 19 publications

References 47 publications

Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Impact of preparation method on nickel speciation and methane dry reforming performance of Ni/SiO2 catalysts

Highly Efficient Ni-Phyllosilicate Catalyst with Surface and Interface Confinement for CO₂ and CO Methanation

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Three-dimensional flower-like nickel phyllosilicates for CO2methanation: enhanced catalytic activity and high stability

Abstract: A group of MCF-derived nickel phyllosilicates were designed and synthesized by a hydrothermal method for enhanced CO2 methanation.

Cited by 19 publications

References 47 publications

Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Synthesis and Regeneration of Ni-Phyllosilicate Catalysts Using a Versatile Double-Accelerator Method: A Comprehensive Study

Impact of preparation method on nickel speciation and methane dry reforming performance of Ni/SiO2 catalysts

Highly Efficient Ni-Phyllosilicate Catalyst with Surface and Interface Confinement for CO2 and CO Methanation

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Three-dimensional flower-like nickel phyllosilicates for CO₂methanation: enhanced catalytic activity and high stability

Highly Efficient Ni-Phyllosilicate Catalyst with Surface and Interface Confinement for CO₂ and CO Methanation