Article
Chemistry, Multidisciplinary
Sushma A. Rawool, Rajesh Belgamwar, Rajkumar Jana, Ayan Maity, Ankit Bhumla, Nevzat Yigit, Ayan Datta, Gunther Rupprechter, Vivek Polshettiwar
Summary: By using magnesium as a catalyst, CO2 can be converted into methane, methanol and formic acid without the need for external energy input. The reaction occurs at 300K and 1 bar within a few minutes, with hydrogen being the predominant product. The cooperative action of magnesium, basic magnesium carbonate, CO2, and water is essential for this transformation, and any missing component will result in the inhibition of the CO2 conversion process.
Article
Engineering, Environmental
B. S. Xaba, A. S. Mahomed, H. B. Friedrich
Summary: The experiments on Ga2O3 and ZrO2 modified Cu-Zn based catalysts revealed that the ZrO2 promoted catalyst showed higher methanol productivity. Furthermore, the ZrO2 modified catalyst exhibited advantages in CO2 uptake and adsorption strength, contributing to the higher methanol yield.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Construction & Building Technology
Xiangping Xian, Yixin Shao
Summary: This study found that ambient pressure carbonation can achieve comparable carbon uptake and strength gain as high pressure carbonation at both early and late age, making it more economic and practical for precast products. Nitrogen adsorption/desorption results revealed that ambient pressure performed better than high pressure in reducing the cumulative pore volume and refining the capillary pore size.
CONSTRUCTION AND BUILDING MATERIALS
(2021)
Article
Physics, Applied
Beomgyun Jeong, Dooyong Lee, Ji-In Park, Sang Moon Lee
Summary: The study reveals that hydrous Pd oxide shows different spectral features than anhydrous Pd oxide under gaseous water environments, providing new information for better identification of hydrous Pd oxide under reaction conditions that is not available from conventional XPS in ultrahigh vacuum.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Wuyang Liang, Jinsong Fu, Honglin Chen, Xiaoming Zhang, Guowei Deng
Summary: The novel Pd-Ce/AC catalyst demonstrated higher H2O2 productivity and lower hydrogenation capacity compared to Pd/AC catalyst, likely attributed to the reduction in Pd particle size and enhancement of Pd2+ content by the addition of Ce.
Article
Chemistry, Physical
Youngseok Yu, Dooyong Lee, Beomgyun Jeong
Summary: Work function is a crucial parameter for metal surfaces in electronics and catalysis, and it is sensitive to surface chemistry and structure changes. Ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) is a method that allows simultaneous observation of surface chemistry and the corresponding change in work function. This study reveals the relationship between the surface abundance of carbon impurity and the work function of Pt(1 1 1), emphasizing the need for surface cleaning to obtain accurate work functions.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Ritwik Mondal, Ravikumar Thimmappa, Bhojkumar Nayak, Anweshi Dewan, Mruthyunjayachari Chattanahalli Devendrachari, Qingsong Chen, Zhenhai Wen, Musthafa Ottakam Thotiyl
Summary: By harvesting the energy of water formation, contaminated hydrogen streams can be refined to nearly 99.9% purity in a single-step at an expenditure of 24 kJ mol(H2)(-1) and with an electrical energy output of 90 kJ mol(H2)(-1) under ambient conditions. A laboratory-level prototype can spontaneously generate nearly 99.4% pure hydrogen in a single-step, even from a quaternary mixture of impurities that include hydrocarbons, CO2 and N-2.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Juan Liu, Xiaoxiao Guo, Zhaoyuan Lyu, Rong-Bin Song, Pengyu Zhou, Shichao Ding, Yang Zhou, Li-Ping Jiang, Yuehe Lin, Wenlei Zhu
Summary: By using copper electrocatalysts and microorganisms, an electro-bio tandem reactor was designed to convert CO2 into specific multicarbon compounds in both the gas and liquid phases. The reducing products from electrocatalysis can be consumed and recycled for selective acetate synthesis in Moorella thermoacetica. The results showed high faradaic selectivity for acetate in liquid products for Cu-based CO2 electroreduction and high electron conversion rate to ethylene and acetate for microbial electrosynthesis, presenting a green design for CO2 upcycling targeting multicarbon products through the parallel integration of electrocatalysis and fermentation.
Article
Chemistry, Applied
Zhirui Ma, Xu Lian, Kaidi Yuan, Shuo Sun, Chengding Gu, Jia Lin Zhang, Jing Lyu, Jian-Qiang Zhong, Lei Liu, Hexing Li, Wei Chen
Summary: The research reveals that O-2 and CO2 can chemically adsorb on ZnO polar surfaces, leading to band-bending in ZnO, while CO does not have the same effect. The electron-acceptor nature of ZnO surfaces affects the binding energy shift of Zn 2p and O 1s due to surface-bound molecules/atoms.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Aitor Arandia, Jihong Yim, Hassaan Warraich, Emilia Leppakangas, Rene Bes, Aku Lempelto, Lars Gell, Hua Jiang, Kristoffer Meinander, Tiia Viinikainen, Simo Huotari, Karoliina Honkala, Riikka L. Puurunen
Summary: The order of addition of copper and zinc on zirconia has significant effects on the catalytic properties, and the catalyst with zinc deposit after copper impregnation shows superior performance in CO2 hydrogenation to methanol.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Shucheng Shi, Yong Han, Tian Yang, Yijing Zang, Hui Zhang, Yimin Li, Zhi Liu
Summary: The effect of surface structure on the oxidation of copper was investigated using ambient-pressure X-ray photoelectron spectroscopy (APXPS). The results showed that Cu(110) required a higher oxygen pressure than Cu(111) to form Cu2O, which was in contrast with the easy formation of O/Cu overlayer on clean Cu(110). These differences in surface structure were attributed to disparities in the kinetic processes.
Article
Chemistry, Multidisciplinary
Seyedeh Behnaz Varandili, Dragos Stoian, Jan Vavra, Kevin Rossi, James R. Pankhurst, Yannick T. Guntern, Nuria Lopez, Raffaella Buonsanti
Summary: Understanding the compositional and structural features of catalysts controlling selectivity is crucial in chemical reactions. This study leveraged tailored Cu/ZnO precatalysts to identify intrinsic features of CuZn catalysts for CO2 reduction, revealing Cu@CuZn core@shell structures selective for methane and ethanol. Surface alloying and metallic Zn concentration were found to improve ethanol selectivity, with density functional theory explaining the selectivity based on electronic and tandem effects. These findings contribute to the rational tuning of bimetallic catalysts for CO2 reduction towards increased selectivity, especially for alcohols.
Article
Engineering, Chemical
Quang Huy Pham, Eirini Goudeli, Colin A. Scholes
Summary: The use of a membrane reactor in methanol synthesis shows promise in selectively removing products, and three thermally resilient glassy polymeric membranes have demonstrated potential for this application.
JOURNAL OF MEMBRANE SCIENCE
(2023)
Article
Chemistry, Physical
S. Zhai, Y. Luo, Z. Fan, M. Zhou, K. Hou, H. Zhao, M. Hu, Y. Xiao, K. Jin, Y. Zhao, X. Li, Z. Cai
Summary: A new strategy has been designed to enhance the electrochemical performance of supercapacitors and water-splitting electrodes by preparing a composite electrode based on CuS, ZnO, and PCc. The composite electrode exhibits outstanding electrochemical energy storage and electrocatalytic performances, achieving high energy density and reduced energy barriers in the oxygen evolution reaction compared to pure materials. This work may inspire the rational design of composite electrode materials for high performance in cross-field applications.
MATERIALS TODAY ENERGY
(2021)
Article
Engineering, Chemical
Stephen J. A. DeWitt, Ryan P. Lively
Summary: This work discusses the development of a novel metal-organic framework (MOF) fiber adsorbent for sub-ambient CO2 capture. Experimental results demonstrate that the fiber adsorbent has good water stability and high adsorption capacity, making it suitable for CO2 capture in practical applications.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Chemistry, Physical
Satoru Ikemoto, Satoshi Muratsugu, Takanori Koitaya, Mizuki Tada
Summary: The role of chromium in Cr- and Rh-incorporated ceria catalysts was investigated, and it was found that chromium facilitated the dispersion of rhodium species and promoted oxygen transfer from NO to CO, enhancing the efficiency of NO reduction with CO at low temperature.
Article
Chemistry, Physical
Taisuke Ochi, Masahiro Kamada, Takamoto Yokosawa, Kozo Mukai, Jun Yoshinobu, Tomohiro Matsui
Summary: Edge engineering is crucial for both fundamental research and applications, especially in the case of graphene, where the electronic properties of the edge depend on the atomic structure and termination. This study investigates the termination of edges created by hydrogen (H) plasma etching, revealing that the edge is sp2 bonded with only one H atom terminating the edge carbon atom. The results suggest that an ideal atomically precise and sp2 bonded zigzag edge can be achieved through H-plasma etching. Additionally, scanning tunneling microscopy studies show that deuterium (D) plasma anisotropically etches graphite less efficiently but can create defects more efficiently than H-plasma.
Article
Physics, Applied
Shunsuke Tanaka, Yuta Murotani, Shunsuke A. Sato, Tomohiro Fujimoto, Takuya Matsuda, Natsuki Kanda, Ryusuke Matsunaga, Jun Yoshinobu
Summary: In this study, we investigate the second-harmonic generation (SHG) light from a Pt surface under terahertz (THz) pulses in atmosphere. The THz pulse modulated SHG intensity shows a clear time profile of the THz field, similar to conventional electro-optic sampling. Our method offers a simple and gapless sampling technique for broadband THz pulses without the need for power supply, bias voltage, or fabrication process.
APPLIED PHYSICS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Hiroki Nakahara, Akiko Nomura, Shun Tokuda, Mami Okamura, Kiyoshi Fujisawa, Takanori Koitaya, Yasuhiro Yoshida, Shuhei Furukawa, Yutaka Hitomi
Summary: Nanosized mixed-metal zeolitic imidazolate frameworks (ZIFs) exhibit superoxide dismutase (SOD)-like catalytic activity due to their porous nature and numerous copper active sites. These nanoparticles have potent SOD-like activity and exceptional recyclability.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Naoki Nagatsuka, Shota Kamibashira, Noboru Shibata, Takanori Koitaya, Kazuya Watanabe
Summary: In this study, the coadsorption of oxygen atoms and water molecules on Pt(553) was investigated using vibrational sum-frequency generation spectroscopy. The results revealed the formation of hydroxyl species at the steps due to the dissociation of water molecules. The hydrogen bond network of the water and hydroxyl complex was proposed, and the proton configuration of the water network at the terrace was shown to be strongly influenced by oxygen decoration at the step.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Young Hyun Choi, Septia Eka Marsha Putra, Yuichiro Shiozawa, Shunsuke Tanaka, Kozo Mukai, Ikutaro Hamada, Yoshitada Morikawa, Jun Yoshinobu
Summary: The adsorption states and thermal process of methane on a stepped Pt surface were studied using TPD, IRAS, and DFT calculations. The adsorption energy for methane on the step site was found to be higher than that on the terrace site. IRAS spectrum showed distinct peaks for adsorbed methane on the step site, indicating different stretching and deformation modes. DFT calculations suggested that the most stable adsorption structure was a 2H structure with elongated C-H bonds towards the Pt step atom, indicating slight activation of the adsorbed methane.
Article
Chemistry, Multidisciplinary
Yoshiaki Ishihara, Takanori Koitaya, Yuto Hamahiga, Wataru Sugimoto, Susumu Yamamoto, Iwao Matsuda, Jun Yoshinobu, Ryo Nouchi
Summary: This study reports on the successful induction and electrical detection of methane oxidation reaction at room temperature using IrO2 nanosheets. The electrical resistance of the atomically thin IrO2 nanosheet films decreases upon exposure to methane and disappears when simultaneously exposed to oxygen, indicating the oxidation of methane using lattice oxygen of the nanosheets. The ability of IrO2 nanosheets to oxidize methane down to 300 K is confirmed, making it an important example of monitoring chemical reactions using electrical resistance changes.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Physical
Fumihiko Ozaki, Shunsuke Tanaka, Younghyun Choi, Wataru Osada, Kozo Mukai, Mitsuaki Kawamura, Masahiro Fukuda, Masafumi Horio, Takanori Koitaya, Susumu Yamamoto, Iwao Matsuda, Taisuke Ozaki, Jun Yoshinobu
Summary: Sulfur vacancies on an MoS2 basal plane significantly affect device performance and catalytic activity. This study investigates the electronic states of sulfur vacancies using AP-XPS and density functional theory calculations. The results provide insights into the changes in electronic states induced by sulfur vacancy formation and offer guidance for sulfur vacancy engineering.
Article
Chemistry, Physical
Takanori Koitaya, Kohei Yamamoto, Tomoya Uruga, Toshihiko Yokoyama
Summary: Operandospectroscopy is a powerful technique for characterizing heterogeneous catalysts under working conditions. In this study, ambient-pressure hard X-ray photoelectron spectroscopy (AP-HAXPES) was used to investigate an industrial copper-zinc-alumina methanol synthesis catalyst. The results revealed the surface chemical states and adsorbed intermediates during the catalytic reaction. The findings provide valuable insights into the dynamic behavior of heterogeneous catalysts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Physics, Multidisciplinary
Yuta Murotani, Natsuki Kanda, Tomohiro Fujimoto, Takuya Matsuda, Manik Goyal, Jun Yoshinobu, Yohei Kobayashi, Takashi Oka, Susanne Stemmer, Ryusuke Matsunaga
Summary: We experimentally investigate the origin of the anomalous Hall conductivity in Cd3As2, a three-dimensional Dirac semimetal, driven by circularly polarized light. Our results show that direct photocurrent generation assisted by the terahertz electric field dominates, while the contribution from the Floquet-Weyl nodes is minor when the driving light is in resonance with interband transitions. We propose a generally applicable classification of microscopic mechanisms for light-induced anomalous Hall conductivity.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Tokuhisa Kawawaki, Yusuke Mitomi, Naoki Nishi, Ryuki Kurosaki, Kazutaka Oiwa, Tomoya Tanaka, Hinoki Hirase, Sayuri Miyajima, Yoshiki Niihori, D. J. Osborn, Takanori Koitaya, Gregory F. Metha, Toshihiko Yokoyama, Kenji Iida, Yuichi Negishi
Summary: We have recently discovered [Pt-17(CO)(12)(PPh3)(8)](z) (Pt = platinum; CO = carbon monoxide; PPh3 = triphenylphosphine; z = 1+ or 2+) as a Pt nanocluster that can be synthesized with atomic precision in air. Our study demonstrates the preparation of a Pt-17-supported carbon black (CB) catalyst (Pt-17/CB) with 2.1 times higher oxygen reduction reaction (ORR) activity than commercial Pt nanoparticles/CB. This achievement is attributed to the appropriate electronic structure of the surface Pt atoms of Pt-17/CB, as suggested by density functional theory calculation.
Article
Chemistry, Multidisciplinary
Yasuyuki Yamada, Kentaro Morita, Takuya Sugiura, Yuka Toyoda, Nozomi Mihara, Masanari Nagasaka, Hikaru Takaya, Kiyohisa Tanaka, Takanori Koitaya, Naoki Nakatani, Hiroko Ariga-Miwa, Satoru Takakusagi, Yutaka Hitomi, Toshiji Kudo, Yuta Tsuji, Kazunari Yoshizawa, Kentaro Tanaka
Summary: A biomimetic catalyst based on a mu-nitrido-bridged iron phthalocyanine dimer stacked onto a graphite surface showed high catalytic methane oxidation activity, even at room temperature. The activity was almost 50 times higher than other molecule-based catalysts and comparable to certain natural enzymes in the presence of H2O2. The stacking of the catalyst onto graphite facilitated electron transfer from methane, leading to enhanced catalytic activity.
