Evolution of zincian malachite synthesis by low temperature co-precipitation and its catalytic impact on the methanol synthesis

Zwiener, Leon; Girgsdies, Frank; Brennecke, Daniel; Teschner, Detre; Machoke, Albert G. F.; Schlögl, Robert; Frei, Elias

doi:10.1016/j.apcatb.2019.02.023

Cited by 43 publications

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“…[49,64] Significant efforts are made to develop the new synthetic strategies that could likely replace the state-of-the-art "coprecipitation" route in order to achieve better physicochemical properties of the Cu/ZnO based catalysts. The comparison of the physicochemical properties of the catalysts derived from different techniques [14,16,[68][69][70][71][72] with the present IS method has been summarized in brief in Table 2. It is noteworthy that the catalysts prepared from phase pure zM precursor exhibit high SA Cu and smaller crystallite size of CuO as compared to those of the rest of the systems.…”

Section: Structure and Properties Of Cuo/zno Catalyst Prepared By Calmentioning

confidence: 99%

“…Hence, it is of great interest to develop a new method for synthesis of Cu/ZnO catalyst from the Zn rich phase pure (Cu 1− x ,Zn x ) 2 (OH) 2 CO 3 precursor. Recently, Frei and co‐workers found that low temperature coprecipitation could lead to the increase in the Zn substitution in zinc malachite up to x =0.31.…”

Section: Introductionmentioning

confidence: 99%

“…[9][10][14][15] Hence, the preparation of phase-pure zinc malachite has gained an increasing interest for its outstanding activity. [16] The dispersion of Cu is primarily responsible for the catalytic performance of the Cu based catalysts and there exists a linear relationship between activity and the surface area of Cu. The Cu/ZnO synergy is mainly attributed to the promotion of strong metal support interaction (SMSI) and the improvement of the higher dispersion of the catalytically active copper phase.…”

Section: Introductionmentioning

confidence: 99%

“…The synergy between Cu and ZnO was further demonstrated quantitatively by characterization of the catalysts treated with syngas at 250°C. Recently, Frei and co-workers [16] found that low temperature coprecipitation could lead to the increase in the Zn substitution in zinc malachite up to x = 0.31.In the present work, we are introducing an exclusive directional isomorphous substitution (IS) method to derive Cu/ ZnO catalyst from phase pure precursor, viz., malachite comprising Zn substitution as high as 50 %. Herein, the first [a] Dr.…”

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confidence: 99%

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confidence: 99%

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Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

et al. 2020

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A new methodology has been demonstrated for the synthesis of a series of phase pure (Cu1−x,Znx)2(OH)2CO3 precursors by isomorphous substitution of Zn2+ in the malachite structure. By following the present protocol, it was possible to synthesize the pure phase (Cu1−x,Znx)2(OH)2CO3 with substitution level as high as x=0.5, which is better than the maximum possible value achieved by coprecipitation method, i. e. x=0.31. The isomorphous substitution by Zn2+ leads to the change in the morphology of malachite crystals from flake‐like to regular needle‐like shape with high Zn dispersion. The activity of the calcined catalysts was increased by ∼1.5–1.7 fold for the hydrogenation of syngas to methanol as compared with those prepared from the traditional coprecipitation route. The synergy between Cu and ZnO was further demonstrated quantitatively by characterization of the catalysts treated with syngas at 250 °C.

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Section: Structure and Properties Of Cuo/zno Catalyst Prepared By Calmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

et al. 2020

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Effect of turbulence in micro‐reactors on ultrafast competitive reactions in Cu‐Zn co‐precipitation

Jiang

Chen

et al. 2021

AIChE Journal

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The enhancement of turbulence was considered to be able to bring about better mixing and more uniform distribution of concentration generally, but its influence on ultrafast competitive reactions is an open question. Cu‐Zn co‐precipitation was carried out in three types of micro‐reactors and the turbulent intensity was regulated by changing flow rate and ultrasound power, respectively. Energy‐dispersive spectrometer of precipitates and characteristic aging time indicate the best uniformity of Cu‐Zn distribution in precipitates appears at moderate turbulent intensity. The numerical simulation shows the uniformities of precipitation both in time and in space are impacted by mixing simultaneously but with opposite direction, resulting in the appearance of maximum. The unevenness of Cu‐Zn distribution caused by inconsistent reaction rates along the time will be erased during subsequent structural evolution, while that caused by diverse reaction rates at various positions can survive and further affect the structure and performance of catalysts.

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Roles of interaction between components in CZZA/HZSM‐5 catalyst for dimethyl ether synthesis via CO₂ hydrogenation

et al. 2021

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The roles of interaction between two catalyst components in CuO–ZnO–ZrO2–Al2O3 (CZZA)/HZSM‐5 bifunctional catalyst for dimethyl ether (DME) synthesis via carbon dioxide hydrogenation were investigated. It was found that CZZA catalyst showed excellent stability during methanol (MeOH) synthesis for 100 h, while there was a severe loss of catalytic activity in the bifunctional catalyst for DME synthesis. Hence, the effects of different degrees of intimacy of two catalyst components were studied for DME synthesis, including mixed and separated modes. For the mixed mode, the particle size of catalysts and the amount of reaction intermediates were proven to influence the catalyst deactivation. For the separated mode, the catalysts showed rapid deactivation within a short time. Various characterizations indicated that the remarkable deactivation of separated mode was mainly caused by the decrease of copper active centers (e.g., sintering and oxidation) and blockage of acid sites via increased coke deposition on HZSM‐5.

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Evolution of zincian malachite synthesis by low temperature co-precipitation and its catalytic impact on the methanol synthesis

Cited by 43 publications

References 44 publications

Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

Effect of turbulence in micro‐reactors on ultrafast competitive reactions in Cu‐Zn co‐precipitation

Roles of interaction between components in CZZA/HZSM‐5 catalyst for dimethyl ether synthesis via CO₂ hydrogenation

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Evolution of zincian malachite synthesis by low temperature co-precipitation and its catalytic impact on the methanol synthesis

Cited by 43 publications

References 44 publications

Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu1−x,Znx)2(OH)2CO3 Precursor Catalyst for Methanol Synthesis

Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu1−x,Znx)2(OH)2CO3 Precursor Catalyst for Methanol Synthesis

Effect of turbulence in micro‐reactors on ultrafast competitive reactions in Cu‐Zn co‐precipitation

Roles of interaction between components in CZZA/HZSM‐5 catalyst for dimethyl ether synthesis via CO2 hydrogenation

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Product

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Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

Oriented Isomorphous Substitution: An Efficient and Alternative Route to Fabricate the Zn Rich Phase Pure (Cu_1−x,Zn_x)₂(OH)₂CO₃ Precursor Catalyst for Methanol Synthesis

Roles of interaction between components in CZZA/HZSM‐5 catalyst for dimethyl ether synthesis via CO₂ hydrogenation