Optimization and understanding of ZnO nanoarray supported Cu-ZnO-Al2O3 catalyst for enhanced CO2 -methanol conversion at low temperature and pressure

Sun, Jiyu; Liu, Fangyuan; Salahuddin, Usman; Wu, Mudi; Zhu, Chunxiang; Lu, Xingxu; Zhang, Bo; Zhao, Binchao; Xie, Zhiqiang; Ding, Yunjiang; Li, Dongsheng; Nam, Chang‐Yong; Zhang, Fengyuan; Gao, Pu‐Xian

doi:10.1016/j.cej.2022.140559

Cited by 7 publications

(5 citation statements)

References 46 publications

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“…Energy dispersive X-ray spectroscopy (EDS) element mapping results (Figure S15) indicate that the atomic fraction of Cu is larger on the etched ZnO, suggesting the increasing surface area for CO 2 hydrogenation on the interfaces of Cu and ZnO. 41 Furthermore, high-energy facets such as {101̅ m} (m = 0, 1, 2, or 3) and {21̅ 1̅ n} (n = 0, 1, 2, or 3) can contribute to the easy activation of CO 2 on the surface. 42 These semipolar surfaces could help tailor the binding energy of O 1s to enhance the electron transfer between ZnO and Cu nanoparticles as a result of strong metal−support interaction.…”

Section: Resultsmentioning

confidence: 99%

“…At 300 °C and 10 bar, Cu/E-ZnO achieves a remarkably high methanol yield of 112.8 mol/h/kg, more than 2 times that of Cu/ZnO. Energy dispersive X-ray spectroscopy (EDS) element mapping results (Figure S15) indicate that the atomic fraction of Cu is larger on the etched ZnO, suggesting the increasing surface area for CO 2 hydrogenation on the interfaces of Cu and ZnO . Furthermore, high-energy facets such as {101̅ m } ( m = 0, 1, 2, or 3) and {21̅ 1̅ n } ( n = 0, 1, 2, or 3) can contribute to the easy activation of CO 2 on the surface .…”

Section: Resultsmentioning

confidence: 99%

“…After the ZnO seeding, the ZnO nanorod arrays were grown on the honeycomb substrates using the hydrothermal method as elaborated earlier. 41 To start with the Cu loading using a facile dip-coating method, a Cu(NO 3 ) 2 solution of 1 mg/mL was prepared by dissolving 20 mg of Cu(NO 3 ) 2 into 20 mL of dimethylformamide (DMF). A cordierite honeycomb substrate with a size of 0.94 × 0.94 × 1.13 cm grown with ZnO nanoarrays was soaked into 0.998 mL of the Cu(NO 3 ) 2 solution under sonication at 135 W for 1 min.…”

Section: Methodsmentioning

confidence: 99%

“…To crystallize the ZnO seeds, the substrate was then calcined in an electric furnace at 400 °C for 2 h with a ramp rate of 5 °C/min. After the ZnO seeding, the ZnO nanorod arrays were grown on the honeycomb substrates using the hydrothermal method as elaborated earlier …”

Section: Methodsmentioning

confidence: 99%

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Unraveling Anisotropic and Pulsating Etching of ZnO Nanorods in Hydrochloric Acid via Correlative Electron Microscopy

Liu

Zhu

et al. 2023

ACS Nano

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Despite much technical progress achieved so far, the exact surface and shape evolution during wet chemical etching is less unraveled, especially in ionically bonded ceramics. Herein, by using in situ liquid cell transmission electron microscopy, a repeated two-stage anisotropic and pulsating periodic etching dynamic is discovered during the pencil shape evolution of a single crystal ZnO nanorod in aqueous hydrochloric acid. Specifically, the nanopencil tip shrinks at a slower rate along [0001̅] than that along the ⟨101̅0⟩ directions, resulting in a sharper ZnO pencil tip. Afterward, rapid tip dissolution happens due to accelerated etching rates along various crystal directions. Concurrently, the vicinal base region of the original nanopencil tip emerges as a new tip followed by the repeated sequence of tip shrinking and removal. The high-index surfaces, such as {101̅m} (m = 0, 1, 2, or 3) and {21̅ 1̅n} (n = 0, 1, 2, or 3), are found to preferentially expose in different ratios. Our 3D electron tomography, convergent beam electron diffraction, middle-angle bright-field STEM, and XPS results indicate the dissociative Cl– species were bound to the Zn-terminated tip surfaces. Furthermore, DFT calculation suggests the preferential Cl– passivation over the {101̅1} and (0001) surfaces of lower energy than others, leading to preferential surface exposures and the oscillatory variation of different facet etching rates. The boosted reactivity due to high-index nanoscale surface exposures is confirmed by comparatively enhanced chemical sensing and CO2 hydrogenation activity. These findings provide an in-depth understanding of anisotropic wet chemical etching of ionic nanocrystals and offer a design strategy for advanced functional materials.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 2 more Smart Citations

Unraveling Anisotropic and Pulsating Etching of ZnO Nanorods in Hydrochloric Acid via Correlative Electron Microscopy

Liu

Zhu

et al. 2023

ACS Nano

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“…Methanol is a potential raw material for plastics and other chemical products that entail methanol-to-olefin synthesis . Although methanol is mostly produced from natural gas, production methods that do not involve fossil fuels are under development (for example, electrochemical catalysts, biomasses, and the hydrogenation of CO 2 to methanol (HCM)). − Similar to biomass energy production, HCM is a useful process from a carbon-neutrality perspective, since CO 2 acts as a reusable compound (CO 2 + 3H 2 → CH 3 OH + H 2 O). However, these reactions produce water as a byproduct, and concentrated methanol is required.…”

Section: Introductionmentioning

confidence: 99%

Recovery of Pure Methanol from Humid Gas Using Mn–Co Prussian Blue Analogue

Shudo

Numano

Kawamoto

et al. 2023

ACS Appl. Mater. Interfaces

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Conventional methanol recovery and purification processes are highly energy-intensive; processes using selective adsorbents that consume low energy are preferable. However, conventional adsorbents have low methanol selectivity under humid conditions. In this study, we develop a selective methanol adsorbent, manganese hexacyanocobaltate (MnHCC), which enables the efficient removal of methanol from waste gas and its subsequent reuse. MnHCC adsorbs 4.8 mmol-methanol/g-adsorbent at 25 °C in a humid gas containing 5000 ppmv of methanol, which is five times higher than the adsorption capacity of activated carbon (0.86 mmol/g). Although MnHCC exhibits the simultaneous adsorption of methanol and water, it has a higher adsorption enthalpy for methanol. Thus, pure methanol (95%) was recovered via thermal desorption at 150 °C after dehydration. The estimated energy of this recovery was 18.9 MJ/kg-methanol, approximately half that of existing mass production methods. MnHCC is reusable and stable even after 10 cyclic experiments. Consequently, MnHCC has the potential to contribute to both the recycling of methanol from waste gas and its low-cost purification.

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Enhancing CO2 Hydrogenation to Methanol via Constructing Cu–ZnO–La2O3 Interfaces

Ji,

Lin,

et al. 2023

Catal Lett

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Optimization and understanding of ZnO nanoarray supported Cu-ZnO-Al2O3 catalyst for enhanced CO2 -methanol conversion at low temperature and pressure

Cited by 7 publications

References 46 publications

Unraveling Anisotropic and Pulsating Etching of ZnO Nanorods in Hydrochloric Acid via Correlative Electron Microscopy

Unraveling Anisotropic and Pulsating Etching of ZnO Nanorods in Hydrochloric Acid via Correlative Electron Microscopy

Recovery of Pure Methanol from Humid Gas Using Mn–Co Prussian Blue Analogue

Enhancing CO2 Hydrogenation to Methanol via Constructing Cu–ZnO–La2O3 Interfaces

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