scholarly journals Tuning transition metal carbide activity by surface metal alloying: a case study on CO2capture and activation

2018 ◽  
Vol 20 (34) ◽  
pp. 22179-22186 ◽  
Author(s):  
Martí López ◽  
Luke Broderick ◽  
John J. Carey ◽  
Francesc Viñes ◽  
Michael Nolan ◽  
...  
Keyword(s):  
Transition Metal ◽  
Density Functional ◽  
State Of The Art ◽  
Transition Metal Carbide ◽  
Metal Carbide ◽  
Metal Carbides ◽  
Early Transition Metal ◽  
Transition Metal Carbides ◽  
Surface Metal

The CO2capture and activation on early transition metal carbides can be fine-tuned by surface doping of similar metals as evidenced by state-of-the-art density functional simulations of the adsorption and desorption rates on suited models.

Tuning Transition Metal Carbides Activity by Surface Metal Alloying: Case Study on CO2 Capture and Activation

2018 ◽  
Author(s):  
Marti Lopez ◽  
Luke Broderick ◽  
John J Carey ◽  
Francesc Vines ◽  
Michael Nolan ◽  
...  
Keyword(s):  
Transition Metal ◽  
Co2 Capture ◽  
Density Functional ◽  
Deep Understanding ◽  
Metal Carbides ◽  
Transition Metal Carbides ◽  
Adsorption Sites ◽  
Surface Metal ◽  
A Minor

<div>CO2 is one of the main actors in the greenhouse effect and its removal from the atmosphere is becoming an urgent need. Thus, CO2 capture and storage (CCS) and CO2 capture and usage (CCU) technologies are intensively investigated as technologies to decrease the concentration</div><div>of atmospheric CO2. Both CCS and CCU require appropriate materials to adsorb/release and adsorb/activate CO2, respectively. Recently, it has been theoretically and experimentally shown that transition metal carbides (TMC) are able to capture, store, and activate CO2. To further improve the adsorption capacity of these materials, a deep understanding of the atomic level processes involved is essential. In the present work, we theoretically investigate the possible effects of surface metal doping of these TMCs by taking TiC as a textbook case and Cr, Hf, Mo, Nb, Ta, V, W, and Zr as dopants. Using periodic slab models with large</div><div>supercells and state-of-the-art density functional theory based calculations we show that CO2 adsorption is enhanced by doping with metals down a group but worsened along the d series. Adsorption sites, dispersion and coverage appear to play a minor, secondary constant effect. The dopant-induced adsorption enhancement is highly biased by the charge rearrangement at the surface. In all cases, CO2 activation is found but doping can shift the desorption temperature by up to 135 K.</div>

Tuning Transition Metal Carbides Activity by Surface Metal Alloying: Case Study on CO2 Capture and Activation

2018 ◽  
Author(s):  
Marti Lopez ◽  
Luke Broderick ◽  
John J Carey ◽  
Francesc Vines ◽  
Michael Nolan ◽  
...  
Keyword(s):  
Transition Metal ◽  
Co2 Capture ◽  
Density Functional ◽  
Deep Understanding ◽  
Metal Carbides ◽  
Transition Metal Carbides ◽  
Adsorption Sites ◽  
Surface Metal ◽  
A Minor

<div>CO2 is one of the main actors in the greenhouse effect and its removal from the atmosphere is becoming an urgent need. Thus, CO2 capture and storage (CCS) and CO2 capture and usage (CCU) technologies are intensively investigated as technologies to decrease the concentration</div><div>of atmospheric CO2. Both CCS and CCU require appropriate materials to adsorb/release and adsorb/activate CO2, respectively. Recently, it has been theoretically and experimentally shown that transition metal carbides (TMC) are able to capture, store, and activate CO2. To further improve the adsorption capacity of these materials, a deep understanding of the atomic level processes involved is essential. In the present work, we theoretically investigate the possible effects of surface metal doping of these TMCs by taking TiC as a textbook case and Cr, Hf, Mo, Nb, Ta, V, W, and Zr as dopants. Using periodic slab models with large</div><div>supercells and state-of-the-art density functional theory based calculations we show that CO2 adsorption is enhanced by doping with metals down a group but worsened along the d series. Adsorption sites, dispersion and coverage appear to play a minor, secondary constant effect. The dopant-induced adsorption enhancement is highly biased by the charge rearrangement at the surface. In all cases, CO2 activation is found but doping can shift the desorption temperature by up to 135 K.</div>

scholarly journals Predicting the Effect of Dopants on CO2 Adsorption on Transition Metal Carbides: Case Study on TiC (001)

2020 ◽  
Author(s):  
Marti Lopez ◽  
Francesc Vines ◽  
Michael Nolan ◽  
Frances Illas
Keyword(s):  
Transition Metal ◽  
Transition Metals ◽  
Density Functional ◽  
Transition Metal Carbide ◽  
Metal Carbides ◽  
Functional Theory ◽  
Late Transition Metals ◽  
Late Transition ◽  
Early Transition

Previous work has shown that doping the TiC(001) surface with early transition metals significantly affects CO<sub>2</sub> adsorption and activation which opens a possible way to control this interesting chemistry. In this work we explore other possibilities which include non-transition metals elements (Mg, Ca, Sr, Al, Ga, In, Si, Sn) as well as late transition metals (Pd, Pt, Rh, Ir) and lanthanides (La, Ce) often used in catalysis. Using periodic slab models with large supercells and state-of-the-art density functional theory (DFT) based calculations, we show that, in all the studied cases, CO<sub>2</sub> appears as bent and, hence, activated. However, the effect is especially pronounced for dopants with large ionic crystal radii. These can increase desorption temperature by up to 230K, almost twice the value predicted when early transition metals are used as dopants. However, a detailed analysis of the results shows that the main effect does not come from electronic structure perturbations but from the distortion that the dopant generates into the surface atomic structure. A simple descriptor is proposed that would allow predicting the effect of the dopant on the CO<sub>2</sub> adsorption energy in transition metal carbide surfaces without requiring DFT calculations.

scholarly journals Predicting the Effect of Dopants on CO2 Adsorption on Transition Metal Carbides: Case Study on TiC (001)

2020 ◽  
Author(s):  
Marti Lopez ◽  
Francesc Vines ◽  
Michael Nolan ◽  
Frances Illas
Keyword(s):  
Transition Metal ◽  
Transition Metals ◽  
Density Functional ◽  
Transition Metal Carbide ◽  
Metal Carbides ◽  
Functional Theory ◽  
Late Transition Metals ◽  
Late Transition ◽  
Early Transition

Previous work has shown that doping the TiC(001) surface with early transition metals significantly affects CO<sub>2</sub> adsorption and activation which opens a possible way to control this interesting chemistry. In this work we explore other possibilities which include non-transition metals elements (Mg, Ca, Sr, Al, Ga, In, Si, Sn) as well as late transition metals (Pd, Pt, Rh, Ir) and lanthanides (La, Ce) often used in catalysis. Using periodic slab models with large supercells and state-of-the-art density functional theory (DFT) based calculations, we show that, in all the studied cases, CO<sub>2</sub> appears as bent and, hence, activated. However, the effect is especially pronounced for dopants with large ionic crystal radii. These can increase desorption temperature by up to 230K, almost twice the value predicted when early transition metals are used as dopants. However, a detailed analysis of the results shows that the main effect does not come from electronic structure perturbations but from the distortion that the dopant generates into the surface atomic structure. A simple descriptor is proposed that would allow predicting the effect of the dopant on the CO<sub>2</sub> adsorption energy in transition metal carbide surfaces without requiring DFT calculations.

Catalytic deoxygenation on transition metal carbide catalysts

2016 ◽  
Vol 6 (3) ◽  
pp. 602-616 ◽  
Author(s):  
Mark M. Sullivan ◽  
Cha-Jung Chen ◽  
Aditya Bhan
Keyword(s):  
Transition Metal ◽  
Transition Metal Carbide ◽  
Metal Carbide ◽  
Metal Carbides ◽  
Transition Metal Carbides ◽  
Catalytic Function ◽  
Catalytic Deoxygenation ◽  
Selective Deoxygenation

We highlight the evolution and tunability of catalytic function of transition metal carbides under oxidative and reductive environments for selective deoxygenation reactions.

Transition metal carbide-based materials: synthesis and applications in electrochemical energy storage

2016 ◽  
Vol 4 (27) ◽  
pp. 10379-10393 ◽  
Author(s):  
Ying Xiao ◽  
Jang-Yeon Hwang ◽  
Yang-Kook Sun
Keyword(s):  
Transition Metal ◽  
Electrochemical Energy Storage ◽  
Transition Metal Carbide ◽  
Metal Carbide ◽  
Metal Carbides ◽  
Materials Synthesis ◽  
High Chemical ◽  
Transition Metal Carbides ◽  
The Past ◽  
High Chemical Stability

Transition metal carbides have attracted vast interest over the past years due to their appealing properties such as high conductivity, high chemical stability and thermal stability.

scholarly journals Predicting the Effect of Dopants on CO2 Adsorption in Transition Metal Carbides: Case Study on TiC (001)

2020 ◽  
Vol 124 (29) ◽  
pp. 15969-15976 ◽  
Author(s):  
Martí López ◽  
Francesc Viñes ◽  
Michael Nolan ◽  
Francesc Illas
Keyword(s):  
Transition Metal ◽  
Co2 Adsorption ◽  
Metal Carbides ◽  
Transition Metal Carbides
Sign in / Sign up

Export Citation Format

Share Document