Ultrasmall Ni nanoparticles embedded in Zr-based MOFs provide high selectivity for CO<sub>2</sub> hydrogenation to methane at low temperatures

Zhao, Zhiwei; Zhou, Xiao Yan; Liu, Yanan; Shen, Congcong; Yuan, Cheng‐Zong; Jiang, Yifan; Zhao, Siqi; Ma, Liu-Bo; Cheang, Tuck−Yun; Xu, An‐Wu

doi:10.1039/c8cy00468d

Cited by 88 publications

(50 citation statements)

References 48 publications

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“…19 After the Ni dispersion, the as-synthesized catalyst (as shown in Figure 6c 0 kJ mol −1 , being comparable to the previous reported value (i.e.,~69 kJ mol −1 ). 23 For NTP-catalysis, the method developed by Hicks et al 36 was employed in this study to determine the apparent activation energy (E A, NTP , or the energy barrier) for CO 2 hydrogenation under the NTP conditions. Previous research has shown that the NTP-activated catalysis presents the nonArrhenius behavior likely due to the complex interactions between plasma and catalyst surface.…”

Section: In Situ Drifts Characterization Of Catalytic Co 2 Hydrogenmentioning

confidence: 99%

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Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

Chen

Shao

et al. 2019

AIChE Journal

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A systematic study of Ni supported on metal-organic frameworks (MOFs) catalyst (i.e., 15Ni/UiO-66) for catalytic CO 2 hydrogenation under nonthermal plasma (NTP) conditions was presented. The catalyst outperformed other catalysts based on conventional supports such as ZrO 2 , representing highest CO 2 conversion and CH 4 selectivity at about 85 and 99%, respectively. We found that the turnover frequency of the NTP catalysis system (1.8 ± 0.02 s −1) has a nearly twofold improvement compared with the thermal catalysis (1.0 ± 0.06 s −1). After 20 hr test, XPS and HRTEM characterizations confirmed the stability of the 15Ni/UiO-66 catalyst in the NTPactivated catalysis. The activation barrier for the NTP-activated catalysis was calculated as~32 kJ mol −1 , being lower than the activation energy of the thermal catalysis (~70 kJ mol −1). In situ DRIFTS characterization confirmed the formation of multiple carbonates and formates on catalyst surface activated by NTP, surpassing the control catalysts (e.g., 15Ni/α-Al 2 O 3 and 15Ni/ZrO 2).

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Section: In Situ Drifts Characterization Of Catalytic Co 2 Hydrogenmentioning

confidence: 99%

“…19,21 To date, many metals (e.g., Ru, Pd, and Ni) have been successfully anchored on/into UiO-66 for various catalytic reactions and shown satisfactory catalytic performance. 19,[21][22][23] Although the limited stability of MOFs has been deemed to be a major issue of these materials, 25…”

Section: Introductionmentioning

confidence: 99%

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

Chen

Shao

et al. 2019

AIChE Journal

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“…One such study used a Ni@UiO‐66 catalyst to achieve 100% selectivity of methane for 100 h at 300 °C. [ 80 ] The material was found to possess a 20 wt% nickel loading while the average size of Ni was still ≈2 nm, indicating uniformly dispersed Ni NPs in the core–shell structure. Also, the activation energy of Ni@UiO‐66 was lower than the conventional Ni/ZrO 2 and Ni/SiO 2 catalysts through the Arrhenius plot analysis.…”

Section: Applications Of Ycsns For Heterogeneous Hydrogenation Reactionsmentioning

confidence: 99%

Engineering of Yolk/Core–Shell Structured Nanoreactors for Thermal Hydrogenations

Wang

Price

et al. 2020

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Heterogeneous hydrogenation reactions are of great importance for chemical upgrading and synthesis, but still face the challenges of controlling selectivity and long‐term stability. To improve the catalytic performance, many hydrogenation reactions utilize special yolk/core–shell nanoreactors (YCSNs) with unique architectures and advantageous properties. This work presents the developmental and technological challenges in the preparation of YCSNs that are potentially useful for hydrogenation reactions, and provides a summary of the properties of these materials. The work also addresses the scientific challenges in applications of these YCSNs in various gas and liquid‐phase hydrogenation reactions. The catalyst structures, catalytic performance, structure–performance relationships, reaction mechanisms, and unsolved problems are discussed too. Also, a brief outlook and opportunities for future research in this field are presented. This work on the advancements in YCSNs might inspire the creation of new materials with desired structures for achieving maximal hydrogenation performances.

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“…[ 33,34 ] The processes of photocatalytic CO 2 transformation mainly include the following four crucial steps: light absorption, the adsorption and activation of CO 2 , the separation and migration of photoinduced carriers, and the surface redox reactions, as shown in Figure . [ 9 ] First, the photocatalyst absorbs the photonic energy greater than its bandgap to generate electron−hole pairs and activates the adsorbed CO 2 molecules through the interaction between them. Subsequently, the photoinduced electrons and holes separate from each other and then migrate to the surface active sites.…”

Section: Photocatalytic Co2 Conversionmentioning

confidence: 99%

“…For example, the reaction of CO 2 with hydrogen will produce CH 4 , CH 3 OH, and other hydrocarbons, which can be used as fuels or basic feedstock of petrochemical products. [ 9 ] Alkynyl carboxylic acids or esters, obtained from the reaction between terminal alkyne and CO 2 , have been extensively used in industry and medicine. [ 10 ] The carboxylic cyclization by propargyl alcohol/amine can convert CO 2 into α‐alkylidene cyclic carbonates or oxazolidinones, which are the basic components of plastics and antibiotics respectively.…”

Section: Introductionmentioning

confidence: 99%

The Active Sites Engineering of Catalysts for CO₂ Activation and Conversion

Tang

Wang

2020

Solar RRL

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Catalytic CO2 conversion is considered to be a promising way to simultaneously reduce greenhouse gas emission and realize carbon resource recycling. Several typical reactions including hydrogenation, carboxylation, carboxylic cyclization, and cycloaddition have been extensively studied for yielding high value‐added products. During the process of CO2 conversion, the introduction of light energy and electricity will dramatically lower the energy consumption for CO2 activation so that the whole reaction can efficiently take place at room temperature and atmospheric pressure. For traditional chemical, photochemical, and electrochemical conversions, the processes can be effectively promoted by the rational engineering of active sites on the catalysts. Herein, the most recent advances on the active site engineering of catalysts involving metal or alloy sites, Lewis sites, defect sites, and elemental doping sites are focused on. The influencing mechanisms on the CO2 activation and selective conversion are further discussed according to the structural properties and the interactions with different active sites. Finally, a brief perspective on the future opportunities and challenges in this field is also presented. Researchers who attempt to explore more efficient catalysts for CO2 activation and selective conversion will be guided.

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Ultrasmall Ni nanoparticles embedded in Zr-based MOFs provide high selectivity for CO₂ hydrogenation to methane at low temperatures

Abstract: Highly monodisperse Ni NPs in UiO-66 give both excellent activity and selectivity for CO2 methanation at low temperatures.

Cited by 88 publications

References 48 publications

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

Engineering of Yolk/Core–Shell Structured Nanoreactors for Thermal Hydrogenations

The Active Sites Engineering of Catalysts for CO₂ Activation and Conversion

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Ultrasmall Ni nanoparticles embedded in Zr-based MOFs provide high selectivity for CO2 hydrogenation to methane at low temperatures

Abstract: Highly monodisperse Ni NPs in UiO-66 give both excellent activity and selectivity for CO2 methanation at low temperatures.

Cited by 88 publications

References 48 publications

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO2 hydrogenation

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO2 hydrogenation

Engineering of Yolk/Core–Shell Structured Nanoreactors for Thermal Hydrogenations

The Active Sites Engineering of Catalysts for CO2 Activation and Conversion

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Product

Resources

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Ultrasmall Ni nanoparticles embedded in Zr-based MOFs provide high selectivity for CO₂ hydrogenation to methane at low temperatures

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

Nonthermal plasma (NTP) activated metal–organic frameworks (MOFs) catalyst for catalytic CO₂ hydrogenation

The Active Sites Engineering of Catalysts for CO₂ Activation and Conversion