The dispersed SiO2 microspheres supported Ru catalyst with enhanced activity for ammonia decomposition

Wang, Fang; Liu, Deng; Wu, Ze-Wei; Ji, Kai; Qiao, Chen; Jiang, Xingmao

doi:10.1016/j.ijhydene.2021.03.205

Cited by 27 publications

(9 citation statements)

References 37 publications

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“…Figure 3c listed the NH 3 splitting activity of SA Ni/CeO 2 and advanced catalysts at 300 °C. Figure 3c showed that the H 2 generation rate of NH 3 splitting of SA Ni/CeO 2 (3.544 mmol g −1 min −1 ) was not merely exceed than the best non-noble metal catalysts of Co 25 Mo 45 Ni-10 Fe 10 Cu 10 reported by Hu et al (3.22 mmol g −1 min −1 ), [11] but also outperformed many noble catalysts, e.g., Ru/La 2 O 3 -K (3.12 mmol g −1 min −1 , [34] Ru/SiO 2 -GUS (2.89 mmol g −1 min −1 ), [35] Ru-Cs/CNT(2.32 mmol g −1 min −1 ), [36] Ru/CeO 2 (2.03 mmol g −1 min −1 ), [37] Ru/Pr 2 O 3 (1.9 mmol g −1 min −1 ), [38] Ru/SiC (1.59 mmol g −1 min −1 ), [39] Ru/MgO-DP (1.46 mmol g −1 min −1 ), [40] Ru/Ca(NH 2 ) 2 (0.78 mmol g −1 min −1 ), and Ru-Cs/MgO (0.46 mmol g −1 min −1 ). [41] In addition, the SA Ni/CeO 2 catalyst showed an almost constant H 2 yield of 3.5 mmol g −1 min −1 in a continuous 90-h NH 3 splitting test at 300 °C.…”

Section: Resultsmentioning

confidence: 87%

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Guan

Huang

et al. 2022

Advanced Energy Materials

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With the intense demand for carbon neutralization, [1] green hydrogen (H 2 ) produced by renewable energy has become one of the universal concerns for human society. [2] However, due to low bulk density (0.089 kg m −3 ), which limits the application and transportation of H 2 , the future of H 2 utilization lies in high-density storage. [3] Among diverse high-density hydrogen storage mediums (e.g., CH 4 , CH 3 OH), [4] ammonia (NH 3 ) not only has the advantages of a large hydrogen storage volume density of ≈106 kg m −3 but also zero CO x (CO 2 , CO) emission during the H 2 production process, [5] which is an ideal candidate for constructing the carbon-free hydrogen system. Traditionally, H 2 production from NH 3 splitting is carried out at high temperatures of 600-850 °C, [6,7] and such high operating temperatures cause serious energy consumption and severe corrosion originating from NH 3 . To reduce the reaction temperature, scientists have developed various catalysts, among which Ir and Ru-based catalysts could drive NH 3 splitting at 300 °C with a H 2 produced rate of ≈2 mmol g −1 min −1 at 300 °C. [8] Unfortunately, the expensive and low reserves of these noble metal catalysts restrict their application. [9] Ni is the benchmark and abundant catalyst for NH 3 splitting, [10,11] exhibiting relatively high activity for NH 3 splitting among non-noble metal catalysts. [6,12] Although a series of Ni-based catalysts, e.g., NiMgAl-layered double hydroxides, [13] La and Ce doped Ni catalysts, [14] Ni/molecular sieves heterostructures, [15] Ni-based solid solutions, [16] have been investigated, the highest H 2 production rate of Ni-based catalysts is still limited in ≈4 mmol g −1 min −1 at 600 °C. [16] Therefore, investigating Ni-based catalysts active for NH 3 splitting at low temperature (300 °C) is the key to realizing industrialized NH 3 splitting. [17] Herein, we proposed a Ni single atom catalyst for NH 3 splitting for the first time. Density functional theory disclosed that the atomic Ni sites supported on CeO 2 could significantly weaken the reaction barrier of NH 3 splitting. Further, the Ni single atoms on CeO 2 nanosheets (SA Ni/CeO 2 ) were successfully synthesized, showing the unprecedented ultra-low activation temperature and the high H 2 production rate for NH 3 splitting, even exceeding most of the reported noble metal Catalytic splitting NH 3 to H 2 is one of the foundations for building a carbonfree H 2 energy system but requires NH 3 splitting catalysts that are highly active and durable at low temperatures. Although various non-noble catalysts have been designed, NH 3 splitting still operates at relatively high temperatures (600-850 °C). Herein, theoretical calculations predict that the Ni single atoms can change the bonding mode of NiN from covalent bond to ionic bond to boost the NH 3 splitting activity. Further, Ni single atoms supported on CeO 2 nanosheets (SA Ni/CeO 2 ) are synthesized by the sol-gel method, which exhibits a robust 3.544 mmol g −1 min −1 of H 2 yield speed of NH 3 splitt...

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Section: Resultsmentioning

confidence: 87%

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Guan

Huang

et al. 2022

Advanced Energy Materials

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“…The Ru 3p core level was analyzed to obtain further information regarding the coexistence of the Ru species onto the SiO 2 -based catalysts (Figure A,B). Both materials presented only slight peak shifting; specifically, Ru-Sdc (Ru 0 : 3p 3/2 = 461.2 eV and 3p 1/2 = 483.7 eV; Ru 4+ : 3p 3/2 = 464.1 eV and 3p 1/2 = 487.0 eV) and Ru-Sdp (Ru 0 : 3p 3/2 = 460.8 eV and 3p 1/2 = 483.3 eV; Ru 4+ : 3p 3/2 = 463.8 eV and 3p 1/2 = 486.5 eV). , Also, their O 1s and Si 2p spectra correspond to Si–O bonds (Figure S12). , …”

Section: Resultsmentioning

confidence: 99%

“…Both materials presented only slight peak shifting; specifically, Ru-Sdc (Ru 0 : 3p 3/2 = 461.2 eV and 3p 1/2 = 483.7 eV; Ru 4+ : 3p 3/2 = 464.1 eV and 3p 1/2 = 487.0 eV) and Ru-Sdp (Ru 0 : 3p 3/2 = 460.8 eV and 3p 1/2 = 483.3 eV; Ru 4+ : 3p 3/2 = 463.8 eV and 3p 1/2 = 486.5 eV). 53,54 Also, their O 1s and Si 2p spectra correspond to Si− O bonds (Figure S12). 55,56 However, the analysis of Ru species for TiO 2 −SiO 2 supports in this region is not an easy task as Ti 2p lines partially overlap with the Ru 3p core level.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Correlating O-Vacancy and Hydrogen Spillover with Activity and Selectivity in Furfural Hydrogenation Using Nanocatalysts Comprised of Ru Nanoparticles Supported on TiO₂–SiO₂

Almeida

Bazan

Gastelois

et al. 2023

ACS Appl. Nano Mater.

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The nanoengineering of efficient and stable nanocatalysts is highly desired for sustainable biomass valorization toward the selective hydrogenation of furfural. The interaction of supports with metallic nanoparticles and oxygen vacancies has a significant role in the catalytic activity of oxide nanocatalysts. Here, by combining density functional theory (DFT) calculations and catalytic experimental data, we demonstrated that the presence of TiO 2 in Ru−SiO 2 catalysts might allow an association between oxygen vacancies and the hydrogen spillover effect. Specifically, Ru−TiO 2 −SiO 2 and Ru−SiO 2 nanocatalysts displayed improved activities and selectivities toward the reaction mentioned above. The nanomaterials were prepared by a simple, versatile, and single-step modified sol− gel process build upon two different stabilizing agents (P123 and CTAB), which afforded entirely covered surfaces of TiO 2 −SiO 2 and SiO 2 supports with uniform small Ru nanoparticles generated in situ. The Ru-TSdc nanocatalyst displayed several interesting promising nanoscale features for hydrogenation of furfural: (i) uniform distribution of Ru, Ti, and Si elements over the entire catalyst surface, (ii) deposition of small Ru nanoparticles with no significant particle agglomeration, (iii) facilitated hydrogen spillover from Ru NPs to the TiO 2 support, and (iv) a significant amount of oxygen vacancies at the nanoparticle surface. For these reasons, the Ru-TSdc sample afforded the optimal performance toward the selective hydrogenation of furfural (up to 99% of selectivity), maintaining good conversions in certain reaction conditions. This work demonstrates how the catalytic activity of metallic nanoparticles could be improved by the structural addition of a reducible oxide, leading to more efficient inorganic supports and for preparing nanocatalysts.

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“…Wang et al 127 prepared Cs(K)-promoted Ru/SiO 2 catalysts, and it was found that promoter K and the Cs played different roles in the ammonia decomposition reaction. They demonstrated that introducing K to catalysts was beneficial for NH 3 adsorption, and Cs played a role in modifying the electronic state of ruthenium nanoparticles.…”

Section: Energymentioning

confidence: 99%

Review on Ru-Based and Ni-Based Catalysts for Ammonia Decomposition: Research Status, Reaction Mechanism, and Perspectives

Guan

Zhou

et al. 2023

Energy Fuels

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Hydrogen (H2) is a zero-carbon and high-energy-density fuel promising to replace fossil fuels for power generation and clean energy. However, hydrogen still faces enormous challenges in terms of production, transportation, and storage. Ammonia (NH3) is a promising H2 (17.7 wt %) carrier that easily overcomes the difficulties associated with H2 storage and transport. However, for the NH3 decomposition hydrogen production reaction, the biggest challenge at present is to achieve complete conversion of ammonia under a relatively high space velocity (about 30,000 mL·gcat –1·h–1) at low-temperature conditions (about 350 °C) with reasonable price catalysts. At present, the most efficient ammonia decomposition catalyst is a Ru-based catalyst doped with K, Ba, and Cs and supported on various carbon supports and metal oxides. Otherwise, the catalysts that exhibited the most outstanding activity among non-noble metal catalysts are nickel-based, and because of their low cost, nickel is regarded as a reasonable alternative candidate material for NH3 decomposition. Advances in the study of reaction kinetics of ammonia decomposition reactions and whether the rate-determining step of the ammonia decomposition reaction is the cleavage of the first N–H bond or the desorption of nitrogen gas are also discussed. This review provides a comprehensive consideration of the recent development of Ru-based and Ni-based catalysts and proposed mechanisms of ammonia decomposition on them are examined. The effects of preparation methods, support, and promoters on catalyst activity were studied and theoretical bases for the design of future catalysts are presented. At last, a brief introduction to catalytic membrane reactor technology in recent years is given. This review can serve as a comprehensive work for designing novel catalysts.

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The dispersed SiO2 microspheres supported Ru catalyst with enhanced activity for ammonia decomposition

Cited by 27 publications

References 37 publications

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Correlating O-Vacancy and Hydrogen Spillover with Activity and Selectivity in Furfural Hydrogenation Using Nanocatalysts Comprised of Ru Nanoparticles Supported on TiO₂–SiO₂

Review on Ru-Based and Ni-Based Catalysts for Ammonia Decomposition: Research Status, Reaction Mechanism, and Perspectives

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The dispersed SiO2 microspheres supported Ru catalyst with enhanced activity for ammonia decomposition

Cited by 27 publications

References 37 publications

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Low Temperature Thermal and Solar Heating Carbon‐Free Hydrogen Production from Ammonia Using Nickel Single Atom Catalysts

Correlating O-Vacancy and Hydrogen Spillover with Activity and Selectivity in Furfural Hydrogenation Using Nanocatalysts Comprised of Ru Nanoparticles Supported on TiO2–SiO2

Review on Ru-Based and Ni-Based Catalysts for Ammonia Decomposition: Research Status, Reaction Mechanism, and Perspectives

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Correlating O-Vacancy and Hydrogen Spillover with Activity and Selectivity in Furfural Hydrogenation Using Nanocatalysts Comprised of Ru Nanoparticles Supported on TiO₂–SiO₂