bluuebunny/crossref_metadata_2025_split huggingface dataset:
Mechanism for Generating H2O2 at Water‐Solid Interface by Contact‐Electrification
Authors: Berbille Andy , Li Xiao‐Fen , Su Yusen , Li Shunning , Zhao Xin , Zhu Laipan , Wang Zhong Lin 
Published: July 2023

AbstractThe recent intensification of the study of contact‐electrification at water‐solid interfaces and its role in physicochemical processes lead to the realization that electron transfers during water‐solid contact‐electrification can drive chemical reactions. This mechanism, named contact‐electro‐catalysis (CEC), allows chemically inert fluorinated polymers to act like single electrode electrochemical systems. This study shows hydrogen peroxide (H2O2) is generated from air and deionized water, by ultrasound driven CEC, using fluorinated ethylene propylene (FEP) as the catalyst. For a mass ratio of catalyst to solution of 1:10000, at 20 °C, the kinetic rate of H2O2 evolution reaches 58.87 mmol L−1 gcat−1 h−1. Electron paramagnetic resonance (EPR) shows electrons are emitted in the solution by the charged FEP, during ultrasonication. EPR and isotope labelling experiments show H2O2 is formed from hydroxyl radicals (HO•) or two superoxide radicals (O2•−) generated by CEC. Finally, it is traditionally believed such radicals migrate in the solution by Brownian diffusion prior to reactions. However, ab‐initio molecular dynamic calculations reveal the radicals can react by exchanging protons and electrons through the hydrogen bonds network of water, i.e., owing to the Grotthuss mechanism. This mechanism can be relevant to other systems, artificial or natural, generating H2O2 from air and water.
Enhancing the Biocompatibility of Additively Manufactured Ti‐6al‐4 V Eli with Diamond‐Like Carbon Coating
Authors: Yick Samuel , Reneman Jake , Martin Philip J. , Evans Margaret D.M. , Bean Penelope A. , Söhnel Tilo , Tse Nicholas M. K. , Bendavid Avi 
Published: July 2023

AbstractOrthopedic implants provide patients with an opportunity to regain functionality lost from illness, disease, or injury. Recent advancements in additive manufacturing (AM) techniques have allowed for the increased customization of Ti‐6Al‐4V ELI (extra low interstitials) implants to complement natural variations in the human anatomy. Yet, the low bioactivity of Ti‐6Al‐4 V ELI and possible adverse effects from the leeching of aluminum and vanadium complicate the post‐operation recovery process. In this work, Ti‐6Al‐4 V ELI samples are printed using the electron beam melt technique in two directions and coated with diamond‐like carbon (DLC) to examine whether their biological properties can be improved. By conducting in vitro studies with Saos‐2 osteosarcoma cells, the effects of morphology and surface chemistry are correlated to the bioactivities of the coated and uncoated samples. The outcome of the study suggested that DLC coating is a viable method for controlling the surface bioactivity of a material. It indicates that a carbon coating, along with an appropriate topography, has the potential to promote the proliferation and maturity of bone cells and hence enhance the performance of additively manufactured products in next‐generation biomedical applications.
The Effect of Phosphorylcholine Coatings on Ice Growing and Melting
Authors: Münch Alexander S. , Fritzsche Tina , Göbel Michael , Simon Frank , Uhlmann Petra 
Published: July 2023

AbstractThe creation of novel approaches to reduce the icing of devices is of economic, technical, and ecological interest. Passive deicing approaches based on thin polymer layers show high potential. (Super)hydrophilic films, characterized by high swelling and surface energy, exhibit a self‐lubricating interfacial layer that can influence ice adhesion. For this purpose, a polymer layer consisting of zwitterionic 2‐methacryloyloxyethyl phosphorylcholine (MPC) and glycidyl methacrylate (GMA) is presented and investigated with respect to its icing behavior. The dependence of the swelling behavior of these layers on temperature and a stabilization of the swelling even at low temperatures is shown and can be directly influenced by the grafting conditions, which have a significant impact on the resulting ice thickness and deicing performance. In addition to the formation of a thinner ice layer, the polymer coatings grafted for 16 h are characterized by excellent deicing performance, resulting in consistently very low ice layer thicknesses in repeated icing–deicing cycles compared to the investigated reference SiO2. Due to these properties, the developed film has high application potential as a coating for heat exchangers, as it enables a reduction of the time between defrosting cycles and the distance between the plates, resulting in energy and material savings.
Zeolitic Imidazole Framework Derived Cobalt Phosphide/Carbon Composite and Waste Paper Derived Porous Carbon for High‐Performance Supercapattery
Authors: Sundriyal Shashank , Dubey Prashant , Mansi  , Gupta Bhavana , Holdynski Marcin , Bonarowska Magdalena , Deep Akash , Shrivastav Vishal , Nogala Wojciech 
Published: July 2023

AbstractMetal–organic frameworks (MOFs) derived nanostructures receive immense research focus due to its high porosity, conductivity, and structural tailrolability features. In this work, porous Zeolitic Imidazole Framework‐67 (ZIF‐67) to synthesize cobalt phosphide/carbon composite (ZCoPC) that serves as a positive electrode is utilized. Furthermore, porous and conductive office paper derived carbon (OPC) are utilized as a negative electrode to make a hybrid system. The metalloid characteristics, high conductivity, and good porosity of ZCoPC material makes it a high‐performance battery like electrode. ZCoPC electrode achieves maximum specific capacity of 192.6 mAh g−1 at 1 A g−1 using 1 m potassium hydroxide (KOH) electrolyte. Furthermore, surface and diffusion charge participation investigation are also undergone for ZCoPC electrode that helps in determining the actual charge dynamics occurring in the electrode. In addition, a supercapattery device is assembled using ZCoPC as battery electrode and OPC as supercapacitor electrode. The as fabricated OPC//ZCoPC hybrid supercapattery device delivers extraordinary energy density of 31.6 Wh kg−1 with a power density of 700 W kg−1 and also a long cycle life of 92.3% even after 10,000 charge–discharge cycles. Hence, these outcomes demonstrate that the synergy of porous MOF derived metal phosphide and OPC electrodes are beneficial for supercapattery devices.
Controlling Photoinduced H2 Release from Freestanding Borophane Sheets Under UV Irradiation by Tuning B–H Bonds
Authors: Hikichi Miwa , Takeshita Junpei , Noguchi Natsumi , Ito Shin‐ichi , Yasuda Yukihiro , Ta Luong Thi , Rojas Kurt Irvin M. , Matsuda Iwao , Tominaka Satoshi , Morikawa Yoshitada , Hamada Ikutaro , Miyauchi Masahiro , Kondo Takahiro 
Published: July 2023

AbstractHydrogen boride (HB), a freestanding 2D hydrogenated‐borophene (borophane) polymorph, is synthesized via ion exchange. HB sheets with a B/H atomic ratio of 1.0 are confirmed to contain three‐center–two‐electron B–H–B bonds and two‐center–two‐electron terminal B–H bonds. The optical properties of HB sheets are expected to be tunable by changing the BHB/BH bond ratio, which alters the electronic structure of HB sheets; however, this is not yet achieved. This study demonstrates that controlling the BHB/BH bond ratio in the HB sheets is possible without altering the hydrogen content by adjusting the volume of ion‐exchange resin during synthesis, thus enabling the tuning of the photoinduced H2 release under UV irradiation. Furthermore, the fluorescence intensity correlates with the absorbance ratio of the BHB and BH vibrational modes. Increasing the BHB/BH bond ratio enhances the luminescence intensity, whereas reducing it enhances the photoinduced H2 release rate under UV irradiation. The ability to control the BHB/BH bond ratio of HB sheets provides new avenues for optimizing their properties for various applications, including hydrogen storage and photocatalysis.
Domain Boundary Formation Within an Intercalated Pb Monolayer Featuring Charge‐Neutral Epitaxial Graphene
Authors: Schädlich Philip , Ghosal Chitran , Stettner Monja , Matta Bharti , Wolff Susanne , Schölzel Franziska , Richter Peter , Hutter Mark , Haags Anja , Wenzel Sabine , Mamiyev Zamin , Koch Julian , Soubatch Serguei , Rosenzweig Philipp , Polley Craig , Tautz Frank Stefan , Kumpf Christian , Küster Kathrin , Starke Ulrich , Seyller Thomas , Bocquet Francois C. , Tegenkamp Christoph 
Published: July 2023

AbstractThe synthesis of new graphene‐based quantum materials by intercalation is an auspicious approach. However, an accompanying proximity coupling depends crucially on the structural details of the new heterostructure. It is studied in detail the Pb monolayer structure after intercalation into the graphene buffer layer on the SiC(0001) interface by means of photoelectron spectroscopy, x‐ray standing waves, and scanning tunneling microscopy. A coherent fraction close to unity proves the formation of a flat Pb monolayer on the SiC surface. An interlayer distance of 3.67 Å to the suspended graphene underlines the formation of a truly van der Waals heterostructure. The 2D Pb layer reveals a quasi ten‐fold periodicity due to the formation of a grain boundary network, ensuring the saturation of the Si surface bonds. Moreover, the densely‐packed Pb layer also efficiently minimizes the doping influence by the SiC substrate, both from the surface dangling bonds and the SiC surface polarization, giving rise to charge‐neutral monolayer graphene. The observation of a long‐ranged () reconstruction on the graphene lattice at tunneling conditions close to Fermi energy is most likely a result of a nesting condition to be perfectly fulfilled.
Facet‐Dependent Interfacial and Photoelectrochemical Properties of TiO2 Nanoparticles
Authors: Zabara Mohammed Ahmed , Yarar Kaplan Begüm , Alkan Gürsel Selmiye , Yürüm Alp 
Published: July 2023

AbstractThe photoelectrochemical properties of titanium dioxide (TiO2) nanoparticles are directly related to the presence of certain facets. The synthesis of such particles is challenged using volatile and sensitive precursors utilizing shape capping agents. In this study, an easier two‐step synthesis technique for the preparation of well‐specified morphology TiO2 nanocrystals from TiO2 powder is demonstrated. The facet‐dependent Fermi level and flat band potential of the prepared particles are calculated and their photoelectrochemical properties are investigated by Cu2+ and Pb2+ photo/electrodeposition. From Cu2+ electrodeposition, it is shown that the presence of {100} and {001} facets in cubic morphology facilitates the electrodeposition with progressive nucleation mechanisms, while the presence of {101} facet in octahedral geometry follows instantaneous nucleation mechanisms. The activity of electroreduction is also related to the flat‐band potential which shows the highest activity in Pb2+ electrodeposition for octahedron nanostructure due to the alignment of the reduction potential to the edge of the flat band. Photodeposition of Cu2+ and Pb2+ ions shows identical trends to electrodeposition indicating the facets influence in ion adsorption and structure of the bandgap of morphological TiO2. The findings emphasize the importance of facet‐dependent surface adsorption and bandgap structure designing faceted TiO2 nanoparticles for tailored applications.
Planar Coupled Nanocavities for Efficient Solar Spectrum Engineering
Authors: Jin Shenghao , Yi Fan , Xu Jianming , Wang Boxiang , Zhao Changying 
Published: July 2023

AbstractTailoring the solar spectrum is critical for energy devices including solar cells and colorful radiative coolers, requiring additional photonic structures with manipulation capabilities adaptable to different application circumstances. However, existing photonic structures cannot effectively balance the trade‐offs between these energy devices' primary functionality, coloration, and visible transparency. Here, a series of planar coupled nanocavities (PCNs) are designed and fabricated, which can manipulate the solar spectrum of energy devices more versatilely than conventional planar multilayers. By judiciously designing and tailoring the coupling effect in the PCNs, the transmissive colors of the PCNs can occupy 99.9% of the sRGB area provided the benchmark for window applications is achieved (average visible transmittance, AVT > 25%), while 25.4% of the sRGB area can be covered by the reflective colors of sub‐ambient radiative coolers with PCNs. Moreover, when serving as the semitransparent electrodes of colorful organic solar cells (OSCs), the PCNs can provide a significantly larger color gamut than commonly used multilayered electrodes under different performance benchmarks. Remarkably, the PCNs can even locally break the trade‐offs between the power conversion efficiency (PCE) and AVT and electrode conductivity of the OSCs. The proposed PCNs provide a promising route for delicately tailoring the solar spectrum with simple multilayered structures.
A Universal Assembly Strategy of All‐Inorganic Non‐Layered Perovskite Single Crystals for High‐Responsivity Photodetectors
Authors: Hong Enliu , Li Ziqing , Cao Fa , Deng Xiaolei , Zhang Xinyu , Fang Xiaosheng 
Published: July 2023

AbstractNon‐layered all‐inorganic perovskite single crystals (AIPSCs) have ultralow trap density and exceptional optoelectronic properties, which can be used for developing high‐performance perovskite optoelectronic devices with high efficiency and stability. However, there is a lack of comprehensive insight and universal principles to guide the preparation of high‐quality AIPSCs. Herein, a universal liquid–air interfacial assembly strategy is proposed for synthesizing non‐layered AIPSCs, in virtue of which a series of AIPSCs including whole structural dimensions from 0D to 3D are acquired. Specially, the CsPbI3 AIPSCs exhibit an ultrathin thickness of 40 nm, and the CsPbBr3 AIPSCs show ultra‐narrow PL FWHM of 11 nm. Photodetectors (PDs) based on CsPbBr3 show excellent performance with responsivity up to 120 A W−1 and detectivity exceeding 2 × 1013 Jones. Moreover, vertically integrated heterojunctions of mixed‐dimensions are fabricated, and the 2D/3D heterostructure PDs further display enhanced self‐powered characteristics. This work provides general synthetic guidance toward the synthesis of non‐layered AIPSCs and promotes their application in AIPSCs‐based optoelectronics.
Tunable Photoluminescence of Bismuth‐ and Trivalent‐Lanthanide‐Doped Monolayer Perovskite Oxide Nanosheets
Authors: Awaya Keisuke , Hatakeyama Kazuto , Ida Shintaro 
Published: July 2023

AbstractMulticolor photoluminescent Bi0.4Ln0.1Na0.5Ta2O72− nanosheets (Ln = Eu, Tb, Dy, Sm, La) are prepared by delaminating an Aurivillius‐phase layered perovskite, Bi2.4Ln0.1Na0.5Ta2O9. Both Bi3+ and Ln3+ (except La3+) successfully function as luminescent centers under UV‐light illumination (λex. = 240–340 nm), which result in a photoluminescence color that can be tuned by changing the lanthanide doping. The emission spectra are influenced by pH because the energy distribution to Ln3+ or to Bi3+ is different in acidic or in basic solutions. Freestanding Bi0.4Ln0.1Na0.5Ta2O72− nanosheet membranes are prepared by vacuum filtration, and the relationship between the photoluminescence and structural properties of the nanosheet membranes is investigated. The results indicate that differences in the electron orbitals involved in the photoluminescence of Bi3+ (6s2–6s6p) and Ln3+ (4fn–4fn) influence the responsiveness to changes in the environment surrounding those luminescent centers.
Upconversion Luminescence Reversible Modulation of Photochromic Ba2YTaO6 Double Perovskite Phosphors Toward Anticounterfeiting Application
Authors: Feng Rongbao , Bai Xue , Zi Yingzhu , Song Youyan , Zhao Heping , Cun Yangke , Liu Yue , Qiu Jianbei , Song Zhiguo , Huang Anjun , Xu Zan , Yang Zhengwen 
Published: July 2023

AbstractDouble perovskite (DP) phosphors attract extensive attention due to their potential applications in the field of optoelectronics. Photochromism‐induced luminescence modulation can extend their application fields. However, designing and preparing DP phosphors with expected photochromic and luminescent properties is still challenging. Herein, the photochromic Ba2YTaO6: Yb3+, Er3+, Co2+ DP with upconversion luminescence properties is developed. The color of the sample turns from white to pink upon 254 nm UV light irradiation, which is fast fading upon 473 nm laser illumination. The mechanism of photochromism is related to the formation of color centers, and the doping of Co2+ ions is crucial for the improvement of photochromism, which is from the increasing of traps depth, the oxygen vacancies, and the carrier concentration of the matrix caused by Co2+ doping. The upconversion luminescence of Er3+ ions can be reversibly modulated by the photochromic effect, exhibiting excellent reproducibility and high stability. The potential application of photochromic Ba2YTaO6: Yb3+, Er3+, Co2+ phosphor is demonstrated in the field of anticounterfeiting and three‐dimensional (3D) artwork. This work not only offers insight into the photochromic mechanism of DP but also presents guidance for developing other photochromic DP phosphors.
Laser Promoting Oxygen Vacancies Generation in Alloy via Mo for HMF Electrochemical Oxidation
Authors: Liu Junbo , Tao Shengyang 
Published: July 2023

AbstractIt is well known that nickel‐based catalysts have high electrocatalytic activity for the 5‐hydroxymethylfurfural oxidation reaction (HMFOR), and NiOOH is the main active component. However, the price of nickel and the catalyst's lifetime still need to be solved. In this work, NiOOH containing oxygen vacancies is formed on the surface of Ni alloy by UV laser (1J85‐laser). X‐ray absorption fine structure (XAFS) analyses indicate an interaction between Mo and Ni, which affects the coordination environment of Ni with oxygen. The chemical valence of Ni is between 0 and 2, indicating the generation of oxygen vacancies. Density functional theory (DFT) suggests that Mo can increase the defect energy and form more oxygen vacancies. In situ Raman electrochemical spectroscopy shows that Mo can promote the formation of NiOOH, thus enhancing the HMFOR activity. The 1J85‐laser electrode shows a longer electrocatalytic lifetime than Ni‐laser. After 15 cycles, the conversion of HMF is 95.92%.
Scalable, Patternable Glass‐Infiltrated Ceramic Radiative Coolers for Energy‐Saving Architectural Applications
Authors: Jeon Seung Kyu , Kim June Tae , Kim Min Seong , Kim In Soo , Park Sung Jin , Jeong Hyeondeok , Lee Gil Ju , Kim Yeong Jae 
Published: July 2023

AbstractA huge concern on global climate/energy crises has triggered intense development of radiative coolers (RCs), which are promising green‐cooling technologies. The continuous efforts on RCs have fast‐tracked notable energy‐savings by minimizing solar absorption and maximizing thermal emission. Recently, in addition to spectral optimization, ceramic‐based thermally insulative RCs are reported to improve thermoregulation by suppressing heat gain from the surroundings. However, a high temperature co‐firing process of ceramic‐based thick film inevitably results in a large mismatch of structural parameters between designed and fabricated components, thereby breaking spectral optimization. Here, this article proposes a scalable, non‐shrinkable, patternable, and thermally insulative ceramic RC (SNPT‐RC) using a roll‐to‐roll process, which can fill a vital niche in the field of radiative cooling. A stand‐alone SNPT‐RC exhibits excellent thermal insulation (≈0.251 W m−1 K−1) with flame‐resistivity and high solar reflectance/long‐wave emissivity (≈96% and 92%, respectively). Alternate stacks of intermediate porous alumina/borosilicate (Al2O3‐BS) layers not only result in outstanding thermal and spectral characteristics, causing excellent sub‐ambient cooling (i.e., 7.05 °C cooling), but also non‐shrinkable feature. Moreover, a perforated SNPT‐RC demonstrates its versatility as a breathable radiative cooling shade and as a semi‐transparent window, making it a highly promising technology for practical deployment in energy‐saving architecture.
Controllable and Reproducible Growth of Transition Metal Dichalcogenides by Design of Experiments
Authors: Heiserer Stefan , Eder Peter , Ó Coileáin Cormac , Biba Josef , Stimpel‐Lindner Tanja , Bartlam Cian , Rührmair Ulrich , Duesberg Georg S. 
Published: July 2023

AbstractControllable and reproducible synthesis of 2D materials is crucial for their future applications. Chemical vapor deposition (CVD) promises scalable and high‐quality growth of 2D materials. However, to optimize CVD growth, multiple parameters have to be carefully selected. Design of experiments (DoE) is a consistent and versatile tool to optimize all parameters simultaneously in a controlled way. This study exploits DoE statistical approaches to show how the CVD growth of transition metal dichalcogenides (TMDs) can be optimized, using tungsten disulfide as an example. A designed set of 29 different processes is used to cover the entire parameter space. The resulting growth output is characterized in terms of material morphology for factors such as single crystal size and continuous film size. The nonlinear model used to fit the output as a function of input parameters provides crucial insights into the nontrivial CVD process ensuring easy and systematic growth optimization. The predicted processes show successful optimization with respect to both the resulting material and the process stability. This powerful technique can be adapted for different setups and other TMD materials.
Topochemical Syntheses of Polyarylopeptides Involving Large Molecular Motions: Frustrated Monomer Packing Leads to the Formation of Polymer Blends
Authors: Raju Cijil , Mridula Kozhukunnon , Srinivasan Nikitha , Kunnikuruvan Sooraj , Sureshan Kana M. 
Published: July 2023

AbstractWe report the topochemical syntheses of three polyarylopeptides, wherein triazolylphenyl group is integrated into the backbone of peptide chains. We synthesized three different monomers having azide and arylacetylene as end‐groups from glycine, L‐alanine and L‐valine. We crystallized these monomers and the crystal structures of two of them were determined by single‐crystal X‐ray diffractometry. Due to the steric constraints, both of these monomers crystallized with two molecules, viz. conformers A and B, in the asymmetric unit. Consistently, in both cases, the A‐conformers are antiparallelly π‐stacked and B‐conformers are parallelly slip‐stacked, exploiting weak interactions. Though the arrangements of molecules in the pristine crystals were unsuitable for topochemical reaction, upon heating, they undergo large motion inside the crystal lattice to reach a transient reactive orientation and thereby the self‐sorted conformer stacks react to give a blend of triazole‐linked polyarylopeptides having two different linkages. Due to the large molecular motion inside crystals, the product phase loses its crystallinity.