Article
Chemistry, Multidisciplinary
Xiaomin Cao, Ronglei Fan, Ju Zhou, Cong Chen, Shunshun Xu, Shuai Zou, Wen Dong, Xiaodong Su, Sheng Ju, Mingrong Shen
Summary: The bifunctional NiMoFe/Cu NW core-shell catalyst assembled into a practical solar-driven overall water splitting system achieved an unprecedented solar-to-hydrogen efficiency of 10.99% in neutral electrolytes, thanks to the unique 3D self-supported core-shell architecture and rapid electron/mass transfer properties.
CHEMICAL COMMUNICATIONS
(2022)
Article
Materials Science, Multidisciplinary
Vasu Prasad Prasadam, Ali Margot Huerta Flores, Jean-Nicolas Audinot, Naoufal Bahlawane
Summary: Solar-driven water splitting is a promising way to obtain clean H-2 energy, and the photoelectrochemical approach has attracted significant interest. The oxygen evolution reaction is seen as the stage that limits performance in this technology, highlighting the need for innovative anode materials. Metal oxide semiconductors are relevant in this respect due to their cost-effectiveness and widespread availability. In this study, a combination of chemical vapor deposition and atomic layer deposition was used to synthesize randomly oriented CNT-ZnO core-shell nanostructures, forming a porous coating that adheres well. Compared to directly coated ZnO on Si, the porous structure allows for a larger interface area with the electrolyte, resulting in a 458% increase in photocurrent density under simulated solar light. The photoelectrochemical characterization attributes this performance enhancement to the effective electron withdrawal along the carbon nanotubes (CNTs), leading to a decrease in the onset potential. As for durability, the CNT-ZnO core-shell structure exhibits enhanced photo-corrosion stability for 8 hours under illumination and with a voltage bias.
Article
Chemistry, Multidisciplinary
Xinwei Wen, Xiaoqiang Yang, Shuli Li, Qing Qu, Lei Li
Summary: Here, we propose a universal strategy for synthesizing transition metal oxide/sulfide heterojunctions as highly efficient catalysts. The edge-rich structure, abundant oxygen defects, and variable valence states of the metals enhance the catalytic performance in water electrolysis, providing an effective and economical approach for large scale catalyst synthesis without the need for noble metals.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Engineering, Environmental
Xiaohong Gao, Jieli Chen, Yanhui Yu, Fangyuan Wang, Xiao Wu, Xingbo Wang, Weihua Mao, Jing Li, Wei Huang, Qi Chen, Ruisong Li, Chenghang You, Shaolei Wang, Xinlong Tian, Zhenye Kang
Summary: In this work, core-shell structured nanoarrays (NiTe@FeOOH) were designed and constructed for efficient overall seawater splitting. The catalyst exhibited superior performance in both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), with low overpotentials and excellent durability. The strong interactions between NiTe and FeOOH, as well as the surface charge effect, contribute to its high activity and stability.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Fenglei Shi, Jiaheng Peng, Fan Li, Ningkang Qian, Hao Shan, Peng Tao, Chengyi Song, Wen Shang, Tao Deng, Hui Zhang, Jianbo Wu
Summary: In this study, an optimized nanocube with enhanced corrosion resistance was designed based on in-situ study on nanoscale corrosion kinetics. The modified nanocube (MNC) showed the best stability performance in practical electrochemical stability testing, with a minimal loss in specific and mass activity after accelerated durability test. This work highlights the importance of in-situ study in guiding the design of materials with improved properties for practical applications.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Minghao Xie, Zhiheng Lyu, Ruhui Chen, Min Shen, Zhenming Cao, Younan Xia
Summary: In this study, Pt-Co@Pt octahedral nanocrystals were successfully synthesized with an intermetallic Pt-Co core and an ultrathin Pt shell dominated by {111} facets on the surface. These nanocrystals showed significantly improved catalytic performance towards the oxygen reduction reaction compared to a commercial Pt/C catalyst, with a mass activity 13.4 times higher and a specific activity 29.5 times higher. Importantly, the mass activity of the nanocrystals only decreased by 21% after 30,000 cycles of accelerated durability testing, indicating their outstanding potential as catalysts for ORR and related reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Jihyeok Song, Youngkwang Kim, Hyo Eun Bae, Sun Young Kang, Jongmin Lee, Mohanraju Karuppannan, Yung-Eun Sung, Yong-Hun Cho, Oh Joong Kwon
Summary: This study investigated the synthesis mechanism of a platinum core-carbon shell catalyst and revealed the key factor determining the properties of the catalyst. The results showed that the ratio of carbon precursor to platinum was the decisive factor in determining the properties of the catalyst.
Article
Chemistry, Multidisciplinary
Zhibin Li, Ruoyu Wu, Yuren Wen, Fu-Kuo Chiang, Xiong-Jun Liu, Jing Wang, Rui Li, Hui Wang, Yuan Wu, Suihe Jiang, Xianzhen Wang, Zhao-Ping Lu
Summary: This work presents a novel nanoporous catalyst design with a core-shell structure, utilizing physical metallurgy to create a self-supported Cu core surrounded by a NiO shell on a metallic glass substrate. These noble metal-free catalysts exhibit outstanding hydrogen evolution reaction (HER) performance, with low overpotential, a low Tafel slope and good durability. The strategy used in this study could be applied to fabricate other nanoporous metals, offering a new approach for designing cost-effective electrode materials.
Article
Chemistry, Multidisciplinary
Xueqin Mu, Xiangyao Gu, Shipeng Dai, Jiabing Chen, Yujia Cui, Qu Chen, Min Yu, Changyun Chen, Suli Liu, Shichun Mu
Summary: The Ru single-atom system constructed on an iron-cobalt layered double hydroxide exhibits low overpotentials and high stability, surpassing commercial RuO2. Its mass activity is significantly higher than Ru and FeCo-LDH. The formation of an in situ Ru-O-TM nanocompound promotes O-O coupling and suppresses heteroatomic interface instability.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Physical
Wanli Gao, Juan Perales-Rondon, Jan Michalicka, Martin Pumera
Summary: Electrochemical nitrate reduction reaction (NO3RR) is a promising method for addressing nitrate pollution and an alternative to traditional ammonia production. This study explores the electrocatalytic activity of 3D printed carbon frameworks consisting of carbon black and carbon nanotubes for NO3RR. The 1D carbon framework exhibits higher electrocatalytic activity with a Faradaic efficiency of over 50% at -1.21 V vs. RHE, attributed to synergistic electrocatalytic contributions between carbon nanotubes and metallic impurities. An ultrathin deposit of electrocatalytic manganese oxides is further added to ensure well-defined surfaces for effective NO3RR. This integrated approach shows promise for electrode fabrication and electrochemical NO3RR.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Lin-Wei Chen, Fuxiang He, Ru-Yang Shao, Qiang-Qiang Yan, Peng Yin, Wei-Jie Zeng, Ming Zuo, Lixin He, Hai-Wei Liang
Summary: The study presents a low-Ir core-shell OER electrocatalyst with high activity in acidic media, showing a significantly improved OER performance compared to commercial Ir/C catalyst. The enhanced activity of the IrGa-IMC@IrOx catalysts is attributed to the modified electronic structure of IrOx induced by the intermetallic IrGa core, leading to improved adsorption capacity for O and OH binding and lower energy barrier for OER rate-determining steps.
Article
Nanoscience & Nanotechnology
T. Kavinkumar, Selvaraj Seenivasan, Amarnath T. Sivagurunathan, Yongchai Kwon, Do-Heyoung Kim
Summary: The rational design and development of novel electrode materials with promising nanostructures can effectively improve supercapacitive performance. By using atomic layer deposition, high-performance electrode materials were developed, showing excellent specific capacity and cycling stability. The demonstrated potential of ALD in next-generation supercapacitors is highlighted by the high energy density and exceptional capacity retention of the assembled supercapattery cell.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Samuel M. Dull, Olga Vinogradova, Shicheng Xu, David M. Koshy, Per Erik Vullum, Jan Torgersen, Sebastian Kirsch, Venkatasubramanian Viswanathan, Thomas F. Jaramillo, Fritz B. Prinz
Summary: Better oxygen reduction catalysts are needed to improve the efficiency of proton exchange membrane fuel cells. This study prepared high-activity Pt-Zn alloy catalysts using two different synthetic approaches, and evaluated their activity. One approach introduced Zn to Pt nanoparticles via atomic layer deposition, resulting in a 30% increase in the activity per Pt mass. Density functional theory calculations were used to understand the origin of this enhancement and guide the preparation of an alloy with higher Zn content.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Qing Zeng, Danye Liu, Hui Liu, Lin Xu, Penglei Cui, Dong Chen, Jing Wang, Jun Yang
Summary: This study presents a gold-catalyzed approach for growing subnanometer-thick metal shells on gold cores. By tuning the composition of the ultrathin shell, the lattice strain effect in the core-shell nanostructures can be further optimized, leading to improved catalytic performance in electrochemical reactions.
CELL REPORTS PHYSICAL SCIENCE
(2022)
Article
Nanoscience & Nanotechnology
Qingying Zhu, Guoyong Yang, Limin Tang, Hongwei Mi, Lingna Sun, Qianling Zhang, Libo Deng, Peixin Zhang, Xiangzhong Ren, Yongliang Li
Summary: In order to improve the efficiency of oxygen evolution reaction, researchers synthesized a heterostructured electrocatalyst by depositing iron oxides on carbon cloth via plasma-enhanced atomic layer deposition, and then growing cobalt oxide nanosheet arrays. This electrocatalyst exhibited excellent electrocatalytic performance for OER in alkaline solution. This design and optimization strategy provides a promising way for the synthesis of ideally designed catalytic architectures for energy storage and conversion applications.
Article
Engineering, Environmental
Tofik Ahmed Shifa, Alessandro Gradone, Khabib Yusupov, Kassa Belay Ibrahim, Matteo Jugovac, Polina Makarovna Sheverdyaeva, Johanna Rosen, Vittorio Morandi, Paolo Moras, Alberto Vomiero
Summary: In this study, a highly efficient catalyst for the oxygen evolution reaction (OER) was developed using a CrOx-CuS heterostructure, which exhibited a low over potential and long-term durability.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
S. Kazim, D. Mastrippolito, P. Moras, M. Jugovac, T. Klimczuk, M. Ali, L. Ottaviano, R. Gunnella
Summary: We investigated the challenging CrCl3 surface using photon energy dependent photoemission (PE). By studying the core and valence electrons of cleaved single crystals in either ultra-high vacuum (UHV) or air, we confirmed the atomic composition with respect to the expected bulk atomic structure. The presence of a stable, but only partially ordered Cl-O-Cr surface was revealed by a common spectroscopic denominator. Through analysis of multiplet components, we quantified the electron charge transfer and the reduced crystal field due to the established polarization field. The methodology used in this study can have a significant impact on determining the structure of ordered sub-oxide phases in mono or bi-layer Cr trihalides.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Kassa Belay Ibrahim, Tofik Ahmed Shifa, Paolo Moras, Elisa Moretti, Alberto Vomiero
Summary: A heterointerface catalyst with strong metal support interaction (SMSI) between WMn2O4 and TiO2 is designed for efficient and stable oxygen evolution reaction (OER). The engineered heterointerface exhibits a low onset overpotential and long-term durability.
Article
Multidisciplinary Sciences
Tommaso Caruso, Oreste De Luca, Nicola Melfi, Alfonso Policicchio, Michele Pisarra, Nicolas Godbert, Iolinda Aiello, Eugenia Giorno, Daniela Pacile, Paolo Moras, Fernando Martin, Petra Rudolf, Raffaele Giuseppe Agostino, Marco Papagno
Summary: The synthesis and design of two-dimensional supramolecular assemblies with specific functionalities is a challenging goal in molecule-based electronics. In this study, we report a novel approach to prepare wide highly crystalline molecular assemblies with tunable structural properties. By utilizing the reactivity of carboxylic acid functional moiety and the predictable features of non-polar alkane chains, we successfully synthesized 2D supramolecular assemblies on a Au(111) surface. These assemblies showed a self-limited highly ordered and defect-free two-dimensional single-layer film of micrometer-size, which could be modified in a controlled way by changing the length of the alkane chains.
SCIENTIFIC REPORTS
(2023)
Article
Materials Science, Multidisciplinary
S. Eremeev, O. De Luca, P. M. Sheverdyaeva, L. Ferrari, A. Matetskiy, G. Di Santo, L. Petaccia, C. Crovara, T. Caruso, M. Papagno, R. G. Agostino, Z. S. Aliev, P. Moras, C. Carbone, E. Chulkov, D. Pacile
Summary: Topological insulators with the Fermi level on the Dirac surface state are actively studied. In this study, we investigate the electronic structure of SnBi2Te4 crystal using angle-resolved photoemission spectroscopy and first-principles calculations. Our results show that away from the Brillouin zone center, bulk bands energetically overlap with the Dirac cone at the Fermi level, leading to unwanted contributions to the material's transport properties. Comparisons between experimental and simulated band structures considering defects provide insights on the limitations in the description of the material.
PHYSICAL REVIEW MATERIALS
(2023)
Article
Green & Sustainable Science & Technology
Getachew Solomon, Mojtaba Gilzad Kohan, Raffaello Mazzaro, Matteo Jugovac, Paolo Moras, Vittorio Morandi, Isabella Concina, Alberto Vomiero
Summary: Hierarchical nanostructures composed of NiMoO4 nanorods surrounded by active MoS2 nanosheets on a nickel foam substrate were designed and showed excellent oxygen evolution reaction performance and charge storage capacity, suggesting promising applications in the catalysis field.
ADVANCED SUSTAINABLE SYSTEMS
(2023)
Article
Chemistry, Physical
Getachew Solomon, Marco Lecca, Matteo Bisetto, Mojtaba Gilzad Kohan, Isabella Concina, Marta Maria Natile, Alberto Vomiero
Summary: Researchers have successfully reduced the photo-oxidation of Cu2O nanowires by growing a thin layer of TiO2 protective layer and an amorphous layer of VOx cocatalyst on them. The optimized photoelectrode exhibits excellent stability and high photocurrent density under simulated sunlight, demonstrating the potential of using earth-abundant materials for solar hydrogen production.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
N. Braud, L. Buss, E. Lundgren, L. R. Merte, H. Wallander, J. -O. Krisponeit, A. Locatelli, T. O. Mentes, M. Jugovac, J. I. Flege, J. Falta
Summary: The cleaning process of the bimetallic Pt3Sn(111) surface was investigated using LEEM, mu.-LEED, and XPEEM techniques. Different cleaning procedures under UHV conditions, including sputtering and annealing, were explored. The study demonstrated that a clean and smooth surface with a well-ordered reconstruction can be achieved through sputtering, high-temperature annealing, and careful cooling. Moreover, the Sn concentration in the topmost layers of Pt3Sn(111) can be tailored by adjusting the annealing temperature and cooling rate, resulting in surface structural changes and different reconstructions.
Article
Multidisciplinary Sciences
W. Janus, T. Slezak, M. Slezak, M. Szpytma, P. Drozdz, H. Nayyef, A. Mandziak, D. Wilgocka-Slezak, M. Zajac, M. Jugovac, T. O. Mentes, A. Locatelli, A. Koziol-Rachwal
Summary: We investigated the magnetic properties of antiferromagnetic NiO(001) thin films in the NiO/MgO(d(MgO))/Cr/MgO(001) system with different thicknesses of MgO. X-ray Magnetic Linear Dichroism results showed that the rotation of NiO spins from in-plane towards out-of-plane direction occurred with an increasing d(MgO). Furthermore, we examined the effect of Fe proximity on the magnetic state of NiO in the Fe/NiO/MgO(d(MgO))/Cr/MgO(001) system. The existence of a multidomain state in NiO was confirmed, which resulted from the competition between the ferromagnet/antiferromagnet exchange coupling and strain exerted on the NiO by the MgO buffer layer.
SCIENTIFIC REPORTS
(2023)
Article
Nanoscience & Nanotechnology
Matteo Jugovac, Iulia Cojocariu, Francesca Genuzio, Chiara Bigi, Debashis Mondal, Ivana Vobornik, Jun Fujii, Paolo Moras, Vitaliy Feyer, Andrea Locatelli, Tevfik Onur Mentes
Summary: Vertical stacks of graphene and ferromagnetic layers are predicted to be efficient spin filters, but experimentally observed figures of merit remain below theoretical predictions. Interface contamination caused by an interfacial carbidic buffer layer is found to affect the spin-polarized electronic structure of graphene on a ferromagnetic cobalt substrate. The presence of interfacial carbon leads to the decoupling of graphene from the ferromagnetic support and the suppression of net spin polarization.
ADVANCED ELECTRONIC MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Iulia Cojocariu, Andreas Windischbacher, Daniel Baranowski, Matteo Jugovac, Rodrigo Cezar de Campos Ferreira, Jiri Dolezal, Martin Svec, Jorge Manuel Zamalloa-Serrano, Massimo Tormen, Luca Schio, Luca Floreano, Jan Dreiser, Peter Puschnig, Vitaliy Feyer, Claus M. Schneider
Summary: Molecule-based functional devices can utilize surface-mediated spin state bistability. Unlike conventional spin crossover complexes, different spin states can only be accessed at temperatures below room temperature, and the high-spin state has a relatively short lifetime. However, the prototypical nickel phthalocyanine exhibits different behavior, as direct interaction with a copper metal electrode mediates the coexistence of high and low spin states within a 2D molecular array. The spin state bistability is non-volatile and originates from the surface-induced axial displacement of the functional nickel cores.
Article
Chemistry, Physical
Valeria Milotti, Stefania Cacovich, Davide Raffaele Ceratti, Daniel Ory, Jessica Barichello, Fabio Matteocci, Aldo Di Carlo, Polina M. Sheverdyaeva, Philip Schulz, Paolo Moras
Summary: This study tracks the evolution of the chemical and optoelectronic properties of FAPbBr(3) films under soft X-ray irradiation using photoemission spectroscopy and micro-photoluminescence. Two contrasting processes are observed during irradiation: material degradation and self-healing. The degradation is characterized by the formation of Pb-0 metallic clusters, loss of gaseous Br-2, and decrease and shift of the photoluminescence emission. The recovery of the photoluminescence signal is attributed to self-healing through the re-oxidation of Pb-0 and migration of FA(+) and Br- ions. This degradation/self-healing effect has the potential to extend the lifetime of perovskite-based X-ray detectors.
Article
Microscopy
Lars Buss, Nicolas Braud, Moritz Ewert, Matteo Jugovac, Tevfik Onur Mentes, Andrea Locatelli, Jens Falta, Jan Ingo Flege
Summary: In this study, the growth of monolayer MoSe2 on selenium-intercalated graphene on Ru (0001) was investigated using low energy electron microscopy and micro-diffraction. Real-time observation revealed the nucleation dynamics of MoSe2 islands at the nanoscale. Larger islands were formed by sliding and attachment of multiple nanometer-sized MoSe2 flakes upon annealing. Micro-spot angle-resolved photoemission spectroscopy showed the electronic structure of the heterostructure, indicating no charge transfer between adjacent layers. The observed behavior was attributed to the intercalation of Se at the graphene/Ru(0001) interface. Thus, the proposed heterostructure serves as a model system for studying graphene supported TMD nanostructures.
Article
Microscopy
Sebastian Guenther, Tim Kratky, Juergen Kraus, Paul Leidinger, Patrick Zeller, Alessandro Sala, Francesca Genuzio, Matteo Jugovac, Tevfik Onur Mentes, Andrea Locatelli
Summary: Non-isochromatism in X-ray PhotoEmission Electron Microscopy (XPEEM) may lead to unwanted artifacts in large field of view images. This lack of isochromatism can be caused by factors such as energy dispersion of X-rays on the sample or the presence of dispersive elements in the electron optics of the microscope. However, a versatile correction procedure has been developed that can fully remove this effect and produce true mono-chromatic photoelectron images with improved signal-to-noise ratio.