Journal ArticleDOI
Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts
Byounghoon Lee,Sunghak Park,Minho Kim,Arun Kumar Sinha,Seong Chan Lee,Euiyeon Jung,Woo Je Chang,Kug-Seung Lee,Jeong Hyun Kim,Sung-Pyo Cho,Hyungjun Kim,Ki Tae Nam,Taeghwan Hyeon +12 more
TLDR
The atomic-level design and synthetic strategy provide a platform that facilitates valence control of co-catalyst copper atoms, reversible modulation of the macroscopic optoelectronic properties of TiO2 and enhancement of photocatalytic hydrogen generation activity, extending the boundaries of conventional heterogeneous catalysts.Abstract:
The reversible and cooperative activation process, which includes electron transfer from surrounding redox mediators, the reversible valence change of cofactors and macroscopic functional/structural change, is one of the most important characteristics of biological enzymes, and has frequently been used in the design of homogeneous catalysts. However, there are virtually no reports on industrially important heterogeneous catalysts with these enzyme-like characteristics. Here, we report on the design and synthesis of highly active TiO2 photocatalysts incorporating site-specific single copper atoms (Cu/TiO2) that exhibit a reversible and cooperative photoactivation process. Our atomic-level design and synthetic strategy provide a platform that facilitates valence control of co-catalyst copper atoms, reversible modulation of the macroscopic optoelectronic properties of TiO2 and enhancement of photocatalytic hydrogen generation activity, extending the boundaries of conventional heterogeneous catalysts. Reversible and cooperative activation processes are important characteristics of biological enzymes and can be used in designing catalysts. Highly active TiO2 photocatalysts incorporated with site-specific single copper atoms are now shown to exhibit such a photoactivation process.read more
Citations
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Journal ArticleDOI
Chemical Synthesis of Single Atomic Site Catalysts.
TL;DR: In this review, various synthetic strategies for the synthesis of SASC are summarized with concrete examples highlighting the key issues of the synthesis methods to stabilize single metal atoms on supports and to suppress their migration and agglomeration.
Journal ArticleDOI
Atomic-level tuning of Co-N-C catalyst for high-performance electrochemical H2O2 production.
Euiyeon Jung,Heejong Shin,Byounghoon Lee,Vladimir Efremov,S. H. Lee,Hyeon Seok Lee,Jiheon Kim,Wytse Hooch Antink,Subin Park,Kug-Seung Lee,Sung-Pyo Cho,Jong Suk Yoo,Yung-Eun Sung,Taeghwan Hyeon +13 more
TL;DR: Interestingly, guided by first-principles calculations, it is found that the catalytic properties of the Co–N4 moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic Properties of metalloenzymes.
Journal ArticleDOI
Heterogeneous Single-Atom Photocatalysts: Fundamentals and Applications.
TL;DR: This review hopes that this review will provide some inspiration for the future discovery of the single-atom photocatalysts, manifestly stimulating the development in this emerging research area.
Journal ArticleDOI
Engineering unsymmetrically coordinated Cu-S 1 N 3 single atom sites with enhanced oxygen reduction activity
Huishan Shang,Xiangyi Zhou,Juncai Dong,Ang Li,Xu Zhao,Qinghua Liu,Yue Lin,Jiajing Pei,Zhi Li,Zhuoli Jiang,Danni Zhou,Lirong Zheng,Yu Wang,Jing Zhou,Zhengkun Yang,Rui Cao,Ritimukta Sarangi,Tingting Sun,Xin Yang,Xusheng Zheng,Wensheng Yan,Zhongbin Zhuang,Jia Li,Wenxing Chen,Dingsheng Wang,Jiatao Zhang,Yadong Li +26 more
TL;DR: An unsymmetrical Cu-S1N3 single atom site on porous carbon with high performance in the oxygen reduction reaction is prepared and provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.
Journal ArticleDOI
Single-Atom Catalysts Based on the Metal-Oxide Interaction.
Rui Lang,Rui Lang,Xiaorui Du,Yike Huang,Yike Huang,Xunzhu Jiang,Xunzhu Jiang,Qian Zhang,Qian Zhang,Yalin Guo,Yalin Guo,Liu Kaipeng,Liu Kaipeng,Botao Qiao,Aiqin Wang,Tao Zhang +15 more
TL;DR: In this review, oxide supported single-atom catalysts are discussed about their synthetic procedures, characterizations, and reaction mechanism in thermocatalysis, such as water-gas shift reaction, selective oxidation/hydrogenation, and coupling reactions.
References
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Journal ArticleDOI
Generalized Gradient Approximation Made Simple
TL;DR: A simple derivation of a simple GGA is presented, in which all parameters (other than those in LSD) are fundamental constants, and only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked.
Journal ArticleDOI
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
Journal ArticleDOI
Projector augmented-wave method
TL;DR: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way and can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function.
Journal ArticleDOI
From ultrasoft pseudopotentials to the projector augmented-wave method
Georg Kresse,Daniel P. Joubert +1 more
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Journal ArticleDOI
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.