Journal ArticleDOI
BEP relations for N2 dissociation over stepped transition metal and alloy surfaces.
TLDR
DFT calculations for N2 dissociation on stepped face-centred cubic (211) surface slabs suggest that the manifestation of BEP relations for surface reactions is a general electronic structure effect, and that geometric effects are responsible for the scatter which is normally observed around the BEP line.Abstract:
We present density functional theory (DFT) calculations for N2 dissociation on stepped face-centred cubic (211) surface slabs. By using the same crystal structure, the same adsorption site for atomic nitrogen, and the same transition-state bond length of N2 over a range of pure metal surfaces, a perfectly linear Bronsted–Evans–Polanyi (BEP) relation between the transition-state potential energy and the dissociative chemisorption energy is obtained. The perfect BEP relation, which extends over 12 eV in chemisorption energy, suggests that the manifestation of BEP relations for surface reactions is a general electronic structure effect, and that geometric effects are responsible for the scatter which is normally observed around the BEP line. The BEP relation is also shown to be valid for both surface and bulk alloys. The scatter is, however, larger than for the pure elements. This can be understood as a larger geometrical variance. To analyze the accuracy of the DFT calculations a detailed convergence study is performed for several adsorbates on stepped hexagonal close-packed and face-centred cubic Ru slabs.read more
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The nature of the active site in heterogeneous metal catalysis.
Jens K. Nørskov,Thomas Bligaard,Britt Hvolbæk,Frank Abild-Pedersen,Ib Chorkendorff,Claus H. Christensen +5 more
TL;DR: This tutorial review, of relevance for the surface science and heterogeneous catalysis communities, provides a molecular-level discussion of the nature of the active sites in metal catalysis, and establishes a strict partitioning between the so-called "electronic" and "geometrical" effects.
Journal ArticleDOI
Understanding trends in electrochemical carbon dioxide reduction rates.
Xinyan Liu,Jianping Xiao,Jianping Xiao,Hong-Jie Peng,Xin Hong,Xin Hong,Karen Chan,Jens K. Nørskov,Jens K. Nørskov +8 more
TL;DR: An understanding of trends in electrocatalytic activity for carbon dioxide reduction over different metal catalysts is presented that rationalize a number of experimental observations including the selectivity with respect to the competing hydrogen evolution reaction.
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Stabilizing metal nanoparticles for heterogeneous catalysis
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Journal ArticleDOI
A Graphene Composite Material with Single Cobalt Active Sites: A Highly Efficient Counter Electrode for Dye‐Sensitized Solar Cells
Xiaoju Cui,Jianping Xiao,Yihui Wu,Peipei Du,Rui Si,Huaixin Yang,Huanfang Tian,Jianqi Li,Wen-Hua Zhang,Dehui Deng,Xinhe Bao +10 more
TL;DR: It is reported that the incorporation of single metal active sites attached to the nitrogen atoms in the basal plane of graphene leads to composite materials with superior activity and stability when used as counter electrodes in dye-sensitized solar cells (DSSCs).
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Toward fundamentals of confined catalysis in carbon nanotubes.
TL;DR: The concept of confinement energy is described, which enables prediction of confinement effects on catalytic activities in different reactions, and is anticipated to be applicable to an even broader range of reactions other than redox of metal species, CO hydrogenation, ammonia synthesis and decomposition discussed here.
References
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