scholarly journals Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products

Molecules ◽  
2021 ◽  
Vol 26 (8) ◽  
pp. 2175
Author(s):  
Di Niu ◽  
Cong Wei ◽  
Zheng Lu ◽  
Yanyan Fang ◽  
Bo Liu ◽  
...  
Keyword(s):  
Density Functional ◽  
Catalyst Surface ◽  
Coupling Reaction ◽  
Reduction Reaction ◽  
Functional Theory ◽  
Faradaic Efficiency ◽  
Barrier Energy ◽  
Co Concentration ◽  
Reduction Of Co2 ◽  
Partial Current

The electrochemical carbon dioxide reduction reaction (CO2RR) to C2 chemicals has received great attention. Here, we report the cuprous oxide (Cu2O) nanocubes cooperated with silver (Ag) nanoparticles via the replacement reaction for a synergetic CO2RR. The Cu2O-Ag tandem catalyst exhibits an impressive Faradaic efficiency (FE) of 72.85% for C2 products with a partial current density of 243.32 mA·cm−2. The electrochemical experiments and density functional theory (DFT) calculations reveal that the introduction of Ag improves the intermediate CO concentration on the catalyst surface and meanwhile reduces the C-C coupling reaction barrier energy, which is favorable for the synthesis of C2 products.

Ethylene formation by methane dehydrogenation and C–C coupling reaction on a stoichiometric IrO2 (110) surface – a density functional theory investigation

2015 ◽  
Vol 5 (8) ◽  
pp. 4064-4071 ◽  
Author(s):  
T. L. M. Pham ◽  
E. G. Leggesse ◽  
J. C. Jiang
Keyword(s):  
Density Functional ◽  
Catalyst Surface ◽  
Coupling Reaction ◽  
Direct Conversion ◽  
Efficient Catalyst ◽  
Functional Theory ◽  
Elementary Reactions ◽  
Ethylene Formation ◽  
Conversion Of Methane ◽  
Mild Temperature

The capability to activate methane at mild temperature and facilitate all elementary reactions on the catalyst surface is a defining characteristic of an efficient catalyst especially for the direct conversion of methane to ethylene.

scholarly journals Screening Highly Efficient Hetero-Diatomic Doped PC6 Electrocatalysts For Selective Nitrogen Reduction to Ammonia

2021 ◽  
Author(s):  
Qiuling Jiang ◽  
Yanan Meng ◽  
Kai Li ◽  
Ying Wang ◽  
Zhijian Wu
Keyword(s):  
Density Functional ◽  
Rational Design ◽  
Synergistic Effects ◽  
Reduction Reaction ◽  
Functional Theory ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Highly Efficient ◽  
Metal Atoms ◽  
Transition Metal Atoms

Abstract Searching for highly efficient electrocatalysts toward nitrogen reduction reaction (NRR) is an important but challenging task for nitrogen utilization in industry. Here we have systematically designed a series of hetero-diatomic catalysts (DACs), in which transition metal atoms (Ti, V, Cr, Mn, Fe, Co, and Ni) are dispersed on PC6 monolayer to form AB@PC6 (A, B= Ti, V, Cr, Mn, Fe, Co, and Ni). Employing density functional theory (DFT) calculation, the V and Cr co-doped PC6 monolayer (VCr@PC6) among the 21 AB@PC6 catalysts is the most promising catalyst due to its low limiting potential of -0.41V, relatively low energy barrier, and high ammonia selectivity toward hydrogen evolution reaction (HER). Insights on the high NRR activity of VCr@PC6 are also explored. The synergistic effect in DACs facilitates the electron transfer from metal pairs to PC6 monolayer, as well as suppresses the HER, leading to high selectivity and Faradaic efficiency. This work not only aims to seek the efficient DACs towards N2 reduction but also provides insights towards synergistic effects between hetero-atoms for the rational design of DACs.

scholarly journals Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Mingchuan Luo ◽  
Ziyun Wang ◽  
Yuguang C. Li ◽  
Jun Li ◽  
Fengwang Li ◽  
...  
Keyword(s):  
Density Functional ◽  
Hydrogen Adsorption ◽  
Reduction Reaction ◽  
Liquid Fuels ◽  
Water Dissociation ◽  
Adsorbed Hydrogen ◽  
Functional Theory ◽  
Faradaic Efficiency ◽  
Complementary Approach ◽  
Cu Catalysts

AbstractProducing liquid fuels such as ethanol from CO2, H2O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO2 reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH)x-doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm−2. Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface *HCCOH, a key intermediate whose fate determines branching to ethanol versus ethylene.

scholarly journals Probing the activity of transition metal M and heteroatom N4 co-doped in vacancy fullerene (M–N4–C64, M = Fe, Co, and Ni) towards the oxygen reduction reaction by density functional theory

RSC Advances ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 3174-3182
Author(s):  
Siwei Yang ◽  
Chaoyu Zhao ◽  
Ruxin Qu ◽  
Yaxuan Cheng ◽  
Huiling Liu ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Transition Metal ◽  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Density Functional ◽  
Reduction Reaction ◽  
Functional Theory ◽  
Co Doped

In this study, a novel type oxygen reduction reaction (ORR) electrocatalyst is explored using density functional theory (DFT); the catalyst consists of transition metal M and heteroatom N4 co-doped in vacancy fullerene (M–N4–C64, M = Fe, Co, and Ni).

scholarly journals Catalyzed Ethanol Chemical Looping Gasification Mechanism on the Perfect and Reduced Fe2O3 Surfaces

Energies ◽  
2021 ◽  
Vol 14 (6) ◽  
pp. 1663
Author(s):  
Laixing Luo ◽  
Xing Zheng ◽  
Jianye Wang ◽  
Wu Qin ◽  
Xianbin Xiao ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Reaction Mechanism ◽  
Density Functional ◽  
Oxygen Carrier ◽  
Catalytic Decomposition ◽  
Density Functional Theory Calculations ◽  
Chemical Looping ◽  
Functional Theory ◽  
Barrier Energy ◽  
Gasification Technology

Biomass chemical looping gasification (CLG) is a novel gasification technology for hydrogen production, where the oxygen carrier (OC) transfers lattice oxygen to catalytically oxidize fuel into syngas. However, the OC is gradually reduced, showing different reaction activities in the CLG process. Fully understanding the CLG reaction mechanism of fuel molecules on perfect and reduced OC surfaces is necessary, for which the CLG of ethanol using Fe2O3 as the OC was introduced as the probe reaction to perform density functional theory calculations to reveal the decomposition mechanism of ethanol into the synthesis gas (including H2, CH4, ethylene, formaldehyde, acetaldehyde, and CO) on perfect and reduced Fe2O3(001) surfaces. When Fe2O3(001) is reduced to FeO0.375(001), the calculated barrier energy decreases and then increases again, suggesting that the reduction state around FeO(001) favors the catalytic decomposition of ethanol to produce hydrogen, which proves that the degree of reduction has an important effect on the CLG reaction.

A systematic computational investigations of water splitting and N2 reduction reaction performances of monolayer MBenes

2021 ◽  
Author(s):  
Yuwen Cheng ◽  
Jisheng Mo ◽  
Yongtao Li ◽  
Yan Song ◽  
Yumin Zhang
Keyword(s):  
Density Functional Theory ◽  
Transition Metal ◽  
Water Splitting ◽  
Density Functional ◽  
Reduction Reaction ◽  
Functional Theory ◽  
Energy Conversion And Storage ◽  
Metal Borides ◽  
Potential Applications ◽  
And Storage

Recently, transition metal borides (MBenes, analogous to MXenes) have been attracted interest due to their potential applications in energy conversion and storage. In this work, we performed density functional theory...

scholarly journals A Free Aluminylene with Diverse σ-Donating and Doubly σ/π-Accepting Ligand Features for Transition Metals

2021 ◽  
Author(s):  
Xin Zhang ◽  
Liu Leo Liu
Keyword(s):  
Density Functional Theory ◽  
Coordination Chemistry ◽  
Transition Metals ◽  
Electronic Structures ◽  
Ligand Exchange ◽  
Density Functional ◽  
Reduction Reaction ◽  
Functional Theory ◽  
Metal Centers ◽  
Coordination Behavior

We report herein the synthesis, characterization, and coordination chemistry of a free N-aluminylene, namely a carbazolylaluminylene 2b. This species is prepared via a reduction reaction of the corresponding carbazolyl aluminium diiodide. The coordination behavior of 2b towards transition metal centers (W, Cr) is shown to afford a series of novel aluminylene complexes 3-6 with diverse coordination modes. We demonstrate that the Al center in 2b can behave as: 1. a σ-donating and doubly π-accepting ligand; 2. a σ-donating, σ-accepting and π-accepting ligand; and 3. a σ-donating and doubly σ-accepting ligand. Additionally, we show ligand exchange at the aluminylene center providing access to the modulation of electronic properties of transition metals without changing the coordinated atoms. Investigations of 2b with IDippCuCl (IDipp = 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene) show an unprecedented aluminylene-alumanyl transformation leading to a rare terminal Cu-alumanyl complex 8. The electronic structures of such complexes and the mechanism of the aluminylene-alumanyl transformation are investigated through density functional theory (DFT) calculations.

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