Article
Engineering, Chemical
Yanju Chen, Chao Feng, Wenhong Wang, Zhi Liu, Junxi Li, Chenguang Liu, Yuan Pan, Yunqi Liu
Summary: The electronic structure of Pd catalyst has been regulated by designing bimetallic Pd-Au alloy nanoparticles with electron-rich Pd, which greatly improves the efficiency of electrocatalytic hydrodechlorination. Experimental characterization and theoretical calculation show that electron-rich Pd promotes the desorption of dechlorination products and accelerates the renewal of active sites. This work provides a strategy for electronic structure engineering of Pd-based electrocatalysts, opening a new opportunity for the design of high-performance hydrodechlorination catalysts.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Crystallography
Jonathan Boltersdorf, Asher C. Leff, Gregory T. Forcherio, David R. Baker
Summary: The study explores the sustainable driving of energy-intensive chemical reactions at low temperatures with solar simulated light using gold-palladium bimetallic nanostructures with engineered plasmon-enhanced activity. By preparing a series of alloy and core-shell Au-Pd nanoparticles, the optical and catalytic properties are tailored to enhance energy-intensive chemical reactions via augmented carrier generation/separation and photothermal conversion. The results show that photogenerated holes primarily drive the photo-oxidation of ethanol and selectively cleave C-C bonds on the Au-Pd bimetallic nanocatalysts.
Article
Multidisciplinary Sciences
Xiaoyang Huang, Ouardia Akdim, Mark Douthwaite, Kai Wang, Liang Zhao, Richard J. Lewis, Samuel Pattisson, Isaac T. Daniel, Peter J. Miedziak, Greg Shaw, David J. Morgan, Sultan M. Althahban, Thomas E. Davies, Qian He, Fei Wang, Jile Fu, Donald Bethell, Steven McIntosh, Christopher J. Kiely, Graham J. Hutchings
Summary: This study demonstrates that the reaction rate can be almost doubled by separating the gold and palladium components in bimetallic carbon-supported catalysts. The enhancement is attributed to the coupling of separate redox processes occurring at isolated gold and palladium sites.
Article
Multidisciplinary Sciences
Julian Gargiulo, Matias Herran, Ianina L. Violi, Ana Sousa-Castillo, Luciana P. Martinez, Simone Ezendam, Mariano Barella, Helene Giesler, Roland Grzeschik, Sebastian Schluecker, Stefan A. Maier, Fernando D. Stefani, Emiliano Cortes
Summary: The authors investigate the influence of bimetallic interface design on the photothermal properties of Au/Pd nanostructures. Measurements using thermometry at the single-particle level show that the inclusion of Pd as a shell significantly reduces the photothermal response compared to bare cores, while including Pd as satellites has minimal effect. These results provide insights into the energy conversion processes in plasmon-assisted catalysis.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Organic
Yuki Naganawa, Yumiko Nakajima, Shigeyoshi Sakaki, Hajime Kameo
Summary: The study elucidated two possible pathways for Si-Cl bond activation in Pd-catalyzed coupling reaction, providing insights for rational catalyst design.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Engineering, Environmental
Alkadevi Verma, Shaili Pal, Jyoti Kuntail, Neha Kamal, R. K. Mandal, Indrajit Sinha
Summary: This study investigates the photocatalytic properties of Cu@Ag and Ag@Cu core-shell nanostructures for the reduction of p-nitrophenol by glycerol under dark and visible light conditions. The Cu@Ag nanoparticles showed significantly enhanced plasmonic photocatalytic activity compared to Ag@Cu nanoparticles. Density functional theory calculations and time-dependent density functional theory simulations were used to understand the electronic structure and mechanism of the core-shell nanostructures.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Bishnu P. Khanal, Eugene R. Zubarev
Summary: This study presents a detailed and systematic investigation on the synthesis of uniform Pd shell on single crystalline and pentahedrally twinned gold nanorods. The thickness of the Pd shell was controlled by the supply of Pd(II) ions during the growth process, resulting in the formation of rectangular-shaped Au@Pd bimetallic nanorods with well-defined morphology. Surprisingly, curved asymmetric nanorods were formed when the Pd deposition was carried out on longer gold nanorods, possibly due to lattice mismatch and flexibility issues.
Article
Chemistry, Physical
Dmitrii German, Ekaterina Pakrieva, Ekaterina Kolobova, Sonia A. C. Carabineiro, Marta Stucchi, Alberto Villa, Laura Prati, Nina Bogdanchikova, Vicente Cortes Corberan, Alexey Pestryakov
Summary: This study investigated the effect of noble metal-based catalysts on the selective oxidation of HMF to FDCA, finding that higher FDCA selectivity was achieved when metals were supported on Sibunit carbon. Furthermore, functionalization of the Sibunit carbon surface with HNO3 and NH4OH led to a change in the active states of Pd and Au, resulting in increased FDCA production.
Article
Chemistry, Multidisciplinary
Gauravjyoti D. Kalita, Podma P. Sarmah, Golap Kalita, Pankaj Das
Summary: A facile ligand-assisted approach was used to synthesize bimetallic Au-Pd nanoparticles with a tunable core@shell structure. The Au-Pd materials exhibited superior performance in two important reactions, with the Pd-core-Au-shell structure showing higher activity compared to the Au-core-Pd-shell structure.
NANOSCALE ADVANCES
(2021)
Article
Chemistry, Multidisciplinary
Jaime Ponce-de-Leon, Guillermo Marcos-Ayuso, Juan A. Casares, Pablo Espinet
Summary: An efficient Pd/Cu bimetallic cross-coupling catalysis for fluoroaryl halides and fluoroarenes is reported. The in situ generation of Cu nucleophile through rate-determining C-H activation of highly fluorinated aryls (>=4 F atoms) leads to high selectivity in cross-coupling reactions with minimal formation of homocoupling products.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Nasrin Nouruzi, Mohammad Dinari, Behnam Gholipour, Nazanin Mokhtari, Mustafa Farajzadeh, Sadegh Rostamnia, Mohammadreza Shokouhimehr
Summary: Highly reactive nanocomposites composed of two-dimensional triazine-based covalent organic polymers (COPs), Pd, and Au nanocomponents were reported. Photocatalytic hydrogen production was achieved under visible light illumination, and it exhibited high catalytic performance.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Haiyang Wang, Dongxia Zhang, Ruiyin Zhang, Hao Ma, Huimin Zhang, Ruijuan Yao, Miaomiao Liang, Yuzhen Zhao, Zongcheng Miao
Summary: Nanorod-structured (Au-Pd)/CeO2 catalysts with different Au/Pd ratios were prepared through dealloying and calcination treatment. Characterization techniques were used to study the structure and physicochemical properties. The (Pd0.15-Au0.15)/CeO2 catalyst calcined at 500°C showed the highest catalytic activity for CO oxidation, reaching 50% and 99% conversion temperatures as low as 50°C and 85°C, respectively. This superior catalytic property is attributed to the robust nanorod structure and introduction of Pd and Au.
Article
Nanoscience & Nanotechnology
Beomjoon Jeon, Daeho Kim, Taek-Seung Kim, Han-Koo Lee, Jeong Young Park
Summary: This study investigates the correlation between catalytic synergy and hot electron chemistry in Au-Pd bimetallic nanoparticles. The formation of Au/PdOx interfaces on the bimetallic catalysts enhances their catalytic activity. By engineering the metal-oxide interfaces, the rate of hot electron formation can be observed.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Nusaiba Zaman, Gabrielle Roberts, Johnathan von der Heyde, Abdelkader Kara
Summary: In this study, the effect of size and composition on the properties of bimetallic nanoclusters was investigated. The geometric structures, stabilities, and electronic properties of Agn-1M (M = Au, Co, Cu, Ni, Pd, Pt; n = 3, 9, 15) nanoclusters were analyzed using spin-polarized density functional theory within the generalized gradient approximation. The results showed that doping pure silver clusters with a transition metal atom improved their stability. The properties including formation energy, electronic structure, magnetic moments, and vibrational density of states were evaluated as a function of size and composition. Weak binding and minor geometric changes were observed for the adsorption of selected bimetallic clusters on a hydroxylated alumina substrate, except for Ag8Pt.
Article
Chemistry, Physical
Libo Sun, Xinyuan Ren, Zequn Yin, HeShun Jing, Miao Zhang, Xuerong Zhou, Xun Sun, Huijuan Su, Caixia Qi
Summary: Bimetallic catalysts of Pd-Au supported on TiO2 with traces of Pd were prepared with improved catalytic activities compared to Au/TiO2. The minimal loading of Pd favors Au dispersion and leads to small-sized Au NPs. The presence of Au/Pd interfaces and interaction between Au and Pd results in electron-enriched Au NPs and positively charged Pd, improving the catalytic performance of 0.01%Pd-0.5%Au/TiO2.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Xiao-Li Pei, Pei Zhao, Hitoshi Ube, Zhen Lei, Koichi Nagata, Masahiro Ehara, Mitsuhiko Shionoya
Summary: The asymmetric induction of metal clusters through ligation of chiral ligands allows for the twisting and stabilization of the resulting chiral structure, which has significant implications for the design of asymmetric catalysts and chiroptical materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Akira Ohnuma, Koki Takahashi, Hironori Tsunoyama, Tomoya Inoue, Pei Zhao, Archana Velloth, Masahiro Ehara, Nobuyuki Ichikuni, Masao Tabuchi, Atsushi Nakajima
Summary: This study demonstrates the enhanced catalytic activity of Pt sub-nanoclusters (containing three to nine Pt atoms) based on charge redistribution. These sub-nanoclusters exhibit higher activity compared to standard Pt/C catalysts and could potentially be used as efficient catalysts in future fuel cell technologies.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Shuaifeng Hu, Pei Zhao, Kyohei Nakano, Robert D. J. Oliver, Jorge Pascual, Joel A. A. Smith, Takumi Yamada, Minh Anh Truong, Richard Murdey, Nobutaka Shioya, Takeshi Hasegawa, Masahiro Ehara, Michael B. B. Johnston, Keisuke Tajima, Yoshihiko Kanemitsu, Henry J. J. Snaith, Atsushi Wakamiya
Summary: In this study, it is found that the surface treatment of mixed tin-lead halide perovskite films with piperazine promotes charge extraction, and combined treatment with CPTA reduces hysteresis and improves efficiency and stability of solar cells.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Yutaka Maeda, Rina Morooka, Pei Zhao, Daiki Uchida, Yui Konno, Michio Yamada, Masahiro Ehara
Summary: The stepwise chemical functionalization of single-walled carbon nanotubes (SWNTs) was employed to selectively control site-specific functionalization and photoluminescence (PL). The addition site and the magnitude of the local band gap were found to be controlled by the steric hindrance of the added group and the R value in an (n,m) chiral nanotube.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Charlie Ruffman, Stephanie Lambie, Krista G. G. Steenbergen, Nicola Gaston
Summary: The melting behavior of Ga-In and Ga-Sn surface slabs was studied using periodic density functional theory and ab initio molecular dynamics. The analysis of structure and electronics revealed insights into the properties of these alloys and their potential as CO2 reduction catalysts. The research showed that the melting points of hexa-layer Ga-In and Ga-Sn were lower than pure hexa-layer Ga, attributed to the disruptive effect of the dopants on the Ga network. Molecular dynamics simulations showed that dopants migrated to and accumulated on the surface of the slabs. The positive charge on the surface dopant atoms and the metallic electronic behavior of the liquid alloys suggested good binding sites for CO2 reduction intermediates.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Stephanie Lambie, Krista G. Steenbergen, Nicola Gaston
Summary: Liquid GaPt catalysts with Pt concentrations as low as 1x10(-4) atomic % have been found to exhibit high activity for the oxidation of methanol and pyrogallol under mild reaction conditions. However, the mechanism behind these significant improvements in activity is still unknown. In this study, ab initio molecular dynamics simulations are used to investigate the behavior of GaPt catalysts and their interaction with adsorbates. The results suggest that persistent geometric features can exist in the liquid state, and the presence of Pt dopant may enable the Ga atoms to become catalytically active.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yui Konno, Rina Morooka, Tatsunari Morishita, Pei Zhao, Naoto Miyasaka, Kazuki Ono, Akira Noda, Daiki Uchida, Ren Iwasaki, Michio Yamada, Masahiro Ehara, Yutaka Maeda
Summary: Functionalization of single-walled carbon nanotubes (SWNTs) using a series of bromoalkanes and dibromoalkanes with different tether lengths was investigated. Longer tether lengths (six or more) resulted in SWNT adducts with two new photoluminescence (PL) peaks, while shorter tether lengths (3-5) produced single peaks. The formation mechanism of functionalized adducts was found to be influenced by the tether length, with shorter tethers tending to produce kinetic products.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Pei Zhao, Masahiro Ehara
Summary: This study systematically explored the activation of NO at metal/oxide interfaces using various metal oxide supports and platinum-group metal clusters. The Pt-4 and Rh-4 clusters showed stronger adsorption energies than the Pd-4 cluster, with the α-Al2O3(100) surface showing the lowest adsorption energy. The activation of NO was found to be an exothermic process, except for the Sr3Fe2O7 case, highlighting the importance of the interplay between the metal cluster and oxygen vacancy.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Medicinal
Nicholas B. Smith, Tim Jowett, Diana Yu, Elke Pahl, Anna L. Garden
Summary: The basin-hopping algorithm (BHA) efficiently explores atomic cluster potential energy surfaces through random perturbations and energy minimizations in configuration space. In multifunnel systems, neither of the two modes of the taboo search method significantly improves performance.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Materials Science, Multidisciplinary
Leonardo Hayato Foianesi-Takeshige, Xiao-Li Pei, Pei Zhao, Hitoshi Ube, Zhen Lei, Masahiro Ehara, Mitsuhiko Shionoya
Summary: This study reports a carbon-centered gold cluster with reversible multi-stimuli responsiveness and reveals the relationship between its photophysical properties and ligand conformation through structural analysis and theoretical calculations. Additionally, the study finds that the gold cluster can emit green light even after losing crystallinity, which is a highly promising model compound for understanding the principles governing stimuli-responsiveness in metal clusters.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yutaka Maeda, Yasuhiro Suzuki, Yui Konno, Pei Zhao, Nobuhiro Kikuchi, Michio Yamada, Masaya Mitsuishi, Anh T. N. Dao, Hitoshi Kasai, Masahiro Ehara
Summary: The authors achieved a shift in the photoluminescence wavelength of single-walled carbon nanotubes to 1320 nm by functionalizing them with 1,4-diiodooctafluorobutane. This finding contributes to the development and application of near-infrared light-emitting materials.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zhen Lei, Pei Zhao, Xiao-Li Pei, Hitoshi Ube, Masahiro Ehara, Mitsuhiko Shionoya
Summary: The aim of this study is to metallize and control the photoluminescence properties of a carbon-centered hexagold(I) cluster using N-heterocyclic carbene (NHC) ligands and silver(I) ions. The results show that the photoluminescence of the clusters depends on the rigidity and coverage of the surface structure. Increasing the coverage of silver(I) ions enhances the phosphorescence efficiency.
Review
Chemistry, Multidisciplinary
Yutaka Maeda, Pei Zhao, Masahiro Ehara
Summary: This review summarizes the latest research progress in tailoring the near-infrared photoluminescent properties of single-walled carbon nanotubes through oxidation and alkylation. The emission wavelength of SWCNTs can be controlled in the range of 1100-1320 nm by chemical modification, and recent developments in chiral separation techniques have increased our understanding of the control of emission wavelength by chemical modification of SWCNTs with different chiral indices.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yutaka Maeda, Rina Morooka, Pei Zhao, Michio Yamada, Masahiro Ehara
Summary: The chiral separation of functionalized SWNTs was achieved through thermal treatment, leading to a shift in emission radiation wavelength. This shift is attributed to the competition between rearrangement and elimination reactions.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Junqing Yin, Masahiro Ehara, Shigeyoshi Sakaki
Summary: Single-atom alloys (SAAs) are promising catalysts that can reduce costs without sacrificing activity. The relative stability of SAAs depends on the interaction energy and coverage between different metal atoms. The electronic structures play a significant role in determining the properties of SAAs, with copper and nickel atoms having weaker interaction energies compared to gold and platinum atoms. These findings are important for the design of efficient catalysts.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)