The cost-effective Cu-based catalysts for the efficient removal of acetylene from ethylene: The effects of Cu valence state, surface structure and surface alloying on the selectivity and activity

Zhang, Riguang; Zhang, Jin; Jiang, Zhao; Wang, Qianqian; Fan, Maohong

doi:10.1016/j.cej.2018.06.083

Cited by 41 publications

(19 citation statements)

References 94 publications

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“…Physicochemical characterizations were performed to monitor the changes in the surface structure and surface chemistry as a consequence of repetitive operation, as they govern activity, selectivity, and Faradaic efficiency of the cycled Ni electrode. ,, The QS-XPS measurements, as shown in Figures S10 and a,b, clearly suggest remarkable differentiation in the chemical composition and chemical states of atoms between different samples. As illustrated in the QS-XPS survey spectra (Figure S10), successive cycles showed an increase in the relative abundance of O and a decline in the relative abundance of Ni, verifying the entrapment of more surface O.…”

Section: Resultsmentioning

confidence: 87%

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Zheng

Zhu

Zhang

et al. 2021

Environ. Sci. Technol.

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Electrocatalytic reduction has recently received increasing attention as a method of converting waste nitrate into value-added ammonia, but most studies have focused on complex strategies of catalyst preparation and little has been done in the way of large-scale demonstrations. Herein, we report that in situ activation of a pristine Ni electrode, either on a lab scale or a pilot scale, is effective in facilitating nitrate reduction to ammonia, exhibiting extraordinarily high activity, selectivity, and stability. The self-activated Ni cathode has a robust capacity to reduce nitrate over a wide range of concentrations and achieves great conversion yield, NH4 +–N selectivity, and Faradaic efficiency, respectively, 95.3, 95.5, and 64.4% at 200 mg L–1 NO3 ––N and 97.8, 97.1, and 90.4% at 2000 mg L–1 NO3 ––N, for example. Fundamental research indicates that Ni(OH)2 nanoparticles are formed on the Ni electrode surface upon self-activation, which play crucial roles in governing nitrate reduction reaction (NO3RR) through the atomic H*-mediated pathway and accordingly suppressing hydrogen evolution reaction. More importantly, the self-activated Ni(OH)2@Ni cathode can be easily scaled up to allow large volumes of real industrial wastewater to be processed, successfully transferring nitrate into ammonia with high yields and Faradaic efficiency. This study demonstrates a new, mild, and promising method of cleaning nitrate-laden wastewater that produces ammonia as a valuable byproduct.

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Section: Resultsmentioning

confidence: 87%

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Zheng

Zhu

Zhang

et al. 2021

Environ. Sci. Technol.

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“…A number of alternative approaches have been investigated to improve the catalytic behavior over non-noble metal materials via focusing on the regulation of the electronic structure, , such as the introduction of the second metal or the modification of the organic compound. In the last few years, introducing reducible metal oxide supports (e.g., TiO 2 , Fe 3 O 4 ) to modify the structure of the active metal is also discovered to be a vital regulating drive to improve the intrinsic activity maintaining high selectivity, in which the charge at the metal/oxide interface can be redistributed governing the principles such as energy minimization. , In addition to the electronic effect, with the development of in situ characterization technology and a deeper understanding of the local fine structure of the catalyst, the interface interaction between metal and support is further expanded.…”

Section: Introductionmentioning

confidence: 99%

Interfacial Bifunctional Effect Promoted Non-Noble Cu/Fe_yMgO_x Catalysts for Selective Hydrogenation of Acetylene

Liu

et al. 2021

ACS Catal.

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Non-noble metal-based catalysts are gradually employed for the conversion of the unsaturated carbon−carbon bond, which exhibits improved selectivity but at the expense of catalytic activity. Herein, in this work, an Fe y MgO x -modified Cu interfacial structure with different Cu/Fe ratios was constructed by a structural topotactic transformation of layered double hydroxides, in which Cu-Fe 0.16 MgO x displayed an enhanced catalytic behavior (95% of selectivity at 100% of conversion and turnover frequency (TOF) of 0.048 s −1 ) in selective hydrogenation of acetylene. By virtue of X-ray absorption spectroscopy, reaction kinetic models, and the calculation based on density functional theory on analyzing the Cu-Fe y MgO x interfacial structure, we demonstrated the formation of the low coordinated Cu δ− -Fe 0.16 δ+ MgO x interfacial sites and further unraveled their dual functions. Specifically, the interfacial Cu δ− sites played a role in the activation of acetylene and hydrogen, while the formed intermediate bounded with the interfacial Cu atom and the interfacial Fe atom, respectively, which was favorable for the desorption to produce ethylene instead of over hydrogenation. This study offers a basic understanding on bifunctional interfacial catalysis for the conversion of the unsaturated carbon−carbon bond, which is of constructive significance for the rational design and preparation of supported non-noble metal materials with high efficiency.

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“…All DFT calculations in this study were implemented using the Dmol code , in Materials Studio 8.0. The generalized gradient approximation (GGA) and Perdew–Burke–Ernzerhof (PBE) functionals , were applied to treat the exchange–correlation potential.…”

Section: Methodsmentioning

confidence: 99%

C₂H₂ Selective Hydrogenation to C₂H₄: Engineering the Surface Structure of Pd-Based Alloy Catalysts to Adjust the Catalytic Performance

Zheng

Wang

et al. 2021

J. Phys. Chem. C

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The surface structure of the catalyst is a key factor to affect its catalytic performance toward the targeted reaction. In this work, aiming at revealing the surface structure influences of Pd-based alloy catalysts on the catalytic performance of C 2 H 2 selective hydrogenation, four kinds of surface structures of Pd-based alloy catalysts, including the core−shell Pd nL @M (M = Cu and Ag), the core−shell Pd nL @Pd x M y , the uniform alloy Pd 1 Cu 3 and Pd 1 Ag 1 , and the subsurface structure Pd 1L -M sub are engineered, and the corresponding catalytic performance is fully examined using DFT calculations. Our results reveal that the catalytic performance of C 2 H 2 selective hydrogenation is closely related to the surface structures of Pd-based alloy catalysts; among them, the

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The cost-effective Cu-based catalysts for the efficient removal of acetylene from ethylene: The effects of Cu valence state, surface structure and surface alloying on the selectivity and activity

Cited by 41 publications

References 94 publications

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Interfacial Bifunctional Effect Promoted Non-Noble Cu/Fe_yMgO_x Catalysts for Selective Hydrogenation of Acetylene

C₂H₂ Selective Hydrogenation to C₂H₄: Engineering the Surface Structure of Pd-Based Alloy Catalysts to Adjust the Catalytic Performance

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The cost-effective Cu-based catalysts for the efficient removal of acetylene from ethylene: The effects of Cu valence state, surface structure and surface alloying on the selectivity and activity

Cited by 41 publications

References 94 publications

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Self-Activated Ni Cathode for Electrocatalytic Nitrate Reduction to Ammonia: From Fundamentals to Scale-Up for Treatment of Industrial Wastewater

Interfacial Bifunctional Effect Promoted Non-Noble Cu/FeyMgOx Catalysts for Selective Hydrogenation of Acetylene

C2H2 Selective Hydrogenation to C2H4: Engineering the Surface Structure of Pd-Based Alloy Catalysts to Adjust the Catalytic Performance

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Interfacial Bifunctional Effect Promoted Non-Noble Cu/Fe_yMgO_x Catalysts for Selective Hydrogenation of Acetylene

C₂H₂ Selective Hydrogenation to C₂H₄: Engineering the Surface Structure of Pd-Based Alloy Catalysts to Adjust the Catalytic Performance