bluuebunny/crossref_metadata_2025_split huggingface dataset:
High Adhesive Polyimide Binder for Silicon Anodes of Lithium Ion Batteries
Authors: Zhang Sanpei , Trask Stephen E. , Dunlop Alison , Polzin Bryant , Qin Yan , Jansen Andrew N. , Lu Wenquan 
Published: July 2021

Silicon has been extensively studied as an anode material in lithium-ion batteries due to its extremely high theoretical specific capacity of 3578 mAh/g (assuming Li15Si4 as intermediate product). However, silicon undergoes huge volume variations during repeated discharge and charge, leading to poor electrode mechanical integrity, continual electrolyte decomposition and fast capacity decay. Developing high strength binders in silicon anodes have been considered as an efficient pathway to alleviate various capacity decay pathways.
Currently, lithiated poly acrylic acid (LiPAA) is mostly used as the binder for silicon electrodes due to its strong binding capability and (electro)chemical compatibility with Si and electrolyte. However, cracks at the electrode level can still be observed for the cycled electrodes, which suggests that a stronger binder is required to mitigate volume expansion of Si electrode and hold the particles together. Herein we study the polyimide (PI) materials as the binders for Si anode in an attempt to achieve stable cycling performance. With PI binder, the silicon electrode exhibits a higher tensile strength than that of conventional PAA binder. The strong adhesion of the PI binder suppresses the structural collapse of the Si negative electrode during lithiation/delithiation, enabling high capacity retention and stable cycle life. However, the PI crosslinking process requires high temperature and inert atmosphere, which is a challenge for its practical application. In this work, we explore various PI crosslinking conditions and their effects on electrochemical performance. This work offers us an alternative binder material with high tensile strength for the Si electrode.
Acknowledgement
We gratefully acknowledge the support from the U.S. Department of Energy's Vehicle Technologies Office. This work is conducted under the Cell Analysis, Modeling, and Prototyping (CAMP) Facility at Argonne National Laboratory. Argonne National Laboratory is operated for DOE office of Science by UChicago Argonne, LLC, under contract number DE-AC02-06CH11357.
The Mechanism of Li Plating on Graphite Particles
Authors: Gao Tao , Fraggedakis Dimitrios , Das Supratim , Chueh William C. , Li Ju , Bazant Martin 
Published: July 2021

Lithium ion battery is the mainstream technology that is powering most of mobile applications (consumer electronics, power tools etc.) and in the future, our transportation by electrifying the vehicles. Current lithium ion battery can only support 1C charging (~50 mins for 80% charge), which is much longer than refilling gasoline car ( < 5 min). Extreme fast charging ( <10 min for 80%) is a very attractive technology that can address this problem. However, Li plating happens in graphite at high charge currents or low temperature, which causes battery performance degradation or even safety hazard (short-circuit, thermal runaway and even fire).
The core of addressing Li plating problem lies in understanding its mechanism. Despite Li ion battery has been invented for 30 years, a systematic understanding on the onset and growth of Li in graphite anode is still lacking. In this work, we elucidate the mechanism of Li plating, by investigating the interplay between Li intercalation and Li plating on a single graphite particle using in-situ optical microscopy coupled with electrochemical test. The results show Li plating happens when the surface of graphite saturates which shuts down the intercalation reaction. The saturation can happen much earlier than full lithiation of graphite particle due to solid diffusion limitation, resulting in severe under-utilization. The discovery sheds light on directions and guidelines of materials innovation or electrode design for achieving extreme fast charging.
Greener Rechargeable Lithium-Ion Batteries Using Plasma Processes at Atmospheric Pressure
Authors: Profili Jacopo , Rousselot Steeve , Tomassi Erica , Briqueleur Elsa , Beauchemin Maxime , Aymé-Perrot David , Stafford Luc , Dolle Mickael 
Published: July 2021

Numerous efforts have been made to develop new thin films by using atmospheric pressure plasma process. Complex materials such as nanocomposite thin films [1.2], biodegradable coatings [3] and advanced chemical treatments on complex surfaces [4] have for example been studied.
Recently, we reported the use of an atmospheric pressure dielectric barrier discharge (DBD) to strongly modify the interfacial properties in lithium-ion batteries [5]. This work focuses on the chemical functionalization of composite electrodes used for aqueous electrolyte rechargeable batteries (ARLB). In this presentation, the physicochemical properties of the coating and electrochemical performance of such electrodes are investigated.
Plasma-deposited coatings were then characterized by SEM-EDX, FTIR and XPS. The electrical analysis indicates that the discharge remains stable during the process. This suggests that the substrate slightly affect the physical regime of the gaseous discharge. The SEM analysis of the plasma-treated electrode suggests a homogeneous surface treatment over a wide area. From the FTIR analysis, different chemical groups were highlighted.
Finally, the electrochemical performance of such electrodes was also investigated in a battery operation. Preliminary explanation of the fundamental mechanisms allowing the operation of the battery and ions diffusion through the plasma layer is attempted.
[1] J. Profili et al., Plasma Processes and Polymers, volume13, issue10, October 2016, 981-989
[2] P. Brunet et al., Plasma Processes and Polymers, volume 14, issue12, December 2017, 1700049
[3] M. Laurent et al., Plasma Processes and Polymers, volume 13, issue7, July 2016, 711-721
[4] S. Asadollahi et al., Materials 2019, 12(2), 219
[5] J. Profili et al., ACS Sustainable Chemistry & Engineering 8 (12), 4728-4733
(Invited) Microkinetic Models for Plasma-Catalytic NH3 Synthesis: Effects of Catalyst Material, Gas Temperature and Power Deposition on Rates and Yields
Authors: Engelmann Yannick , Neyts Erik C. , Bogaerts Annemie 
Published: July 2021

We developed microkinetic plasma catalysis models to investigate the plasma-assisted ammonia synthesis on transition metal catalysts in dielectric barrier discharge plasmas. These models aim at gaining insight in the reaction mechanisms and kinetics of plasma-activated species at the catalytic surface. We focus on the effects of vibrational excitations as well as plasma-generated radicals, on the turnover frequencies and equilibrium conversion.
Based on the results of DFT calculations, we built scaling relations for the catalytic conversion of N2 and H2 towards NH3on transition metal catalysts. These scaling relations allow the generation of ‘volcano’ plots that show the logarithm of the turnover frequencies as function of a catalyst descriptor (in our case the binding energy of N). We compare the volcano plots for thermal catalysis with vibrationally-enhanced catalysis and radical-enhanced catalysis in order to investigate how the plasma can most efficiently aid in the catalytic conversion. Careful analysis of reaction flow diagrams shows which pathways are dominant in each of the regimes. We show that Eley-Rideal (ER) mechanisms can become very important in plasmas with high densities of radical species as opposed to thermal conditions where ER is usually considered negligible compared to Langmuir-Hinschelwood. We determined on which catalysts ER mechanisms are most important and how they impact the turnover frequency.
This framework was introduced in a plasma chemistry model in ZDPlasKin to study conversions as function of catalyst material, gas temperature and specific energy input. Model results show the temporal behavior, with the specific role of microdischarge filaments and afterglows, of filamentary plasmas and how catalyst material, gas temperature and specific energy input can induce conversions beyond thermal equilibrium.
The Effect of Cation Doped ZnO Electron Transport Layer for Pure Blue Emitting Zntese/ZnSe/ZnS Quantum Dot Light Emitting Diodes
Authors: Choi Hyung Seok , Kim Yohan , Kim Jiyong , Geßner André , Wedel Armin 
Published: July 2021

Colloidal quantum dot light emitting diodes (QLED) has considered as next generation display technology due to their accurate color information, high brightness, with low process cost, and potential flexible substrates. Red and green QLED achieved nearly the efficiency of theoretical limitation by optimizing quantum dot materials and device architecture with the tremendous efforts of many fellow researchers [1,2]. However, the authentic blue color QLED with high performance and high stability is yet remained as a obstacle for the commercialization. Herein, we report the fabrication of ZnTeSe based blue QLED device with multi shell quantum dots with very high quantum yield over >90% at 443nm with narrow FWHM of 15 nm. The peak wavelength of quantum dot could be tuned with the different Te/Se ratio of the core and the thickness of intermediate ZnSe shell. With the combination of zinc magnesium oxide (ZMO), which is the most common electron transport layer (ETL) for blue QLED, and our highly luminescent blue quantum dot, bright blue QLEDs with the max luminance of 700 cd/m2 in the inverted structure are demonstrated. Moreover, to obtain the better-performed and stable electron transport layer, different cations such as lithium, nickel, aluminum, cerium, erbium and indium-doped zinc oxides were successfully synthesized and studied. we have analyzed the band gap of ZnO can be fine tuned by doping of different cations and the effect of different zinc oxide in the device will be tested in the further study. According to the recent researches of the device stability of blue QLED [3,4], inferior stability of blue QLED is originated from the interface of ETL and quantum dots. I believe that the study of various ETL materials can give us a key to solve the poor lifetime problem of blue QLED.
Reference
1. Li, Y., Hou, X., Dai, X., Yao, Z., Lv, L., Jin, Y., & Peng, X. (2019). Stoichiometry-Controlled InP-Based Quantum Dots: Synthesis, Photoluminescence, and Electroluminescence. Journal of the American Chemical Society, 141(16), 6448–6452.
2. Won, Y.-H., Cho, O., Kim, T., Chung, D.-Y., Kim, T., Chung, H., ... Jang, E. (2019). Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes. Nature, 575(7784), 634–638.
3. Chen, S., Cao, W., Liu, T., Tsang, S.-W., Yang, Y., Yan, X., & Qian, L. (2019). On the degradation mechanisms of quantum-dot light-emitting diodes. Nature Communications, 10(1), 765.
4. Kim, T., Kim, K.-H., Kim, S., Choi, S.-M., Jang, H., Seo, H.-K., ... Jang, E. (2020). Efficient and stable blue quantum dot light-emitting diode. Nature, 586(7829), 385–389.
(Invited) Optoelectronic Application of Colloidal Quatum Dots in Infrared Beyond Si
Authors: Hwang Gyu Weon , Jin Jun Young , Park Taehwan , Jeong Tae Hoon 
Published: July 2021

Among electromagnetic wave spectrum, infrared region has many attractive applications such as a LiDAR, optical communication, telecommunications, thermography, bioimaging, photovoltaics, and night visions. However, the expensive cost of epitaxial III-V semiconductors and the fabrication process hinders the widespread of the infrared technology beyond the silicon absorption range. Colloidal quantum dots have a great potential as an alternative materials for infrared detection. Lead chalcogenide QDs not only have tunable bandgap in infrared region but also have process compatibility with conventional Si ROIC in the device fabrication process, which remarkably reduces fabrication costs. The performance of photodetectors incorporating the lead chalcogenide QDs, however, is suboptimal and needs further improvement. One of the main factors limiting the performance of QD-based photodetectors is a high density of surface defects. QDs inherently have large surface-to-volume ratios and dangling bonds on the surface acted as trap sites. Various methods to reduce surface defects, such as thermal and ligand treatment, have been introduced; however, even after these treatments, QD-based photodetectors still show the relatively low detectivity (D*).
In this work, we demonstrate the various approaches to improve the performance of infrared photodetectors and their results. We focused on the reducing the trap density by the surface treatment of QDs using thermal annealing and chemical treatment in order to improve the device performance. We developed the chemical treatment method for reducing trap states with maintaining the existing ligands. Thermal annealing also can reduce the trap density; however, it sintered QDs by atomic diffusion. We found optimal condition for reducing the surface traps with suppressing sintering. The effects of these treatments were evaluated by the device performance and trap characterization. These approaches improve the bandwidth and the responsivity compared to reference devices. Moreover, we treated the surface of QD layers to show the interfacial effect on the QD devices.
Determination of Rate Equation for the Electrochemical Hydrogenation and Hydrogenolysis of Furfural in Acidic Media over Copper
Authors: May Andrew , Watt Steven , Biddinger Elizabeth J. 
Published: July 2021

The use of electricity from renewable sources allows for carbon neutral electrochemical processes to be operated. One example process is that of the electrochemical hydrogenation and hydrogenolysis of furfural (FF) to furfuryl alcohol (FA) and 2-methylfuran (MF). FA is used as a reactant in making furanic polymers for molds and castings, and MF has been identified as a high octane fuel. The electrochemical reactions of FF to FA and MF occur in parallel in acidic conditions on Cu catalysts. In this work we investigated the reaction mechanism by proposing a set of elementary steps, deriving the corresponding rate equation, and fitting it to the data. A Langmuirian trend was seen in the production rate vs FF concentration data.
Experimentation was done using a catholyte that contained 0.1 or 0.5 M H2SO4 with a concentration of FF between 10 and 120 mM. The potential was first varied in pH 0 with 100 mM FF to determine the Tafel slope and exchange current densities, as well as the range of potential where the reaction is not mass transfer limited. The Tafel region of the system was found to be between -517 mV and -572 mV. To determine the effect of concentration of FF, the applied potential was set to -560 mV vs RHE, where the system is limited by kinetics and not mass transfer. The reaction rates to desired products were found to change from positive order to zero order with respect to FF concentration, showing a Langmuirian trend. It was found that the plateau in the reaction rate was 50% and 58% lower for MF and FA species respectively when the pH was changed from 0 to 1. The reaction rate equation was determined to be the equation that best fit the data across both pH levels.
Low- and Zero-Cobalt Layered Oxide Cathodes for Lithium-Ion Batteries
Authors: Manthiram Arumugam 
Published: July 2021

Lithium-ion batteries have become an integral part of our daily life, powering portable electronic devices. They are in the process of transforming the transportation sector through electrification. They are also being intensively pursued for grid storage of electricity produced from renewable sources. Cost, sustainability, and supply-chain issues are major considerations in employing lithium-ion batteries for electric vehicle (EV) and grid storage applications. In the case of EVs, energy density or driving distance between charges is a critical parameter as well. These considerations have created immense interest to reduce cobalt content or eliminate cobalt altogether in layered oxide cathodes. With this perspective, the research and development trend has been to increase the nickel content and lower the cobalt content in LiNi1-y-xMny-CozO2 (NMC) cathodes. For instance, the industry has been gradually moving from LiCoO2 with 100% Co to NMC-111 with 33% Ni and 33% Co to NMC-622 with 60% Ni and 20% Co to NMC-811 with 80% Ni and 10% Co. While the increase in Ni content offers both an increase in capacity and a reduction in cost, it is also met with serious technical challenges. As the Ni content increases beyond 60%, the cathodes suffer from poor cycle, thermal, and air stabilities. The problems become exponentially challenging as the Ni content increases. This presentation will focus on improving the cycle, thermal, and air stabilities through compositional and controlled synthesis approaches, while reducing the Co content significantly as well as eliminating it altogether to give low- and zero-cobalt layered oxide cathodes with high capacities.
The low- and zero-cobalt layered oxide cathodes are synthesized by a coprecipitation of the hydroxide precursors with appropriate doping, employing a tank reactor, followed by calcining with lithium hydroxide at optimal temperatures under a flowing oxygen atmosphere. As the Ni content increases, the calcining temperature and conditions need to be sensitively controlled to obtain high-quality samples. The presentation will particularly focus on the performance evaluation and a fundamental understanding of the degradation mechanisms with cathodes containing > 90% nickel, including LiNiO2. The electrochemical performances are evaluated with full pouch cells by pairing the cathodes with graphite anode. The bulk and surface instabilities are assessed by employing a suite of advanced analytical methodologies, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), time-of-flight – secondary ion mass spectrometry (TOF-SIMS), high-resolution transmission electron microscopy (HR-TEM), etc. before and after extended cycling of full pouch cells. The presentation will also focus on assessing and improving the air stability as well as thermal stability of various compositions. Approaches to realize capacity values as high as 220 mAh/g will be presented.
(Invited) Mass Transport and Storage in Li-Ion Electrodes: Bulk and Interfaces
Authors: Maier Joachim 
Published: July 2021

The subject of batteries is the interconversion of compositional changes and outer electrical potential changes. In solids all compositional changes refer explicitly to defect chemistry. Point defects such as interstitial and vacancies enable ion transport, mass transport and represent the species affected by storage [1].
The contribution discusses the modes of storage (bulk and interfacial storage) [2], derives the respective theoretical charge/discharge curves and discusses transport kinetics. The latter follow from the defect chemical picture, too. As for storage (chemical capacitance) also for transport (chemical resistance) one may distinguish between bulk and boundary phenomena [3]. The defect-chemical description is shown not only to be the adequate description (superior to, e.g. lattice gas models), it also leads to a generalized picture of electrode and supercapacitive storage.

References

[1] J. Maier, Angewandte Chemie International Edition 52 (2013) 4998.
[2] C.-C. Chen, J. Maier, Nature Energy 3 (2018) 102.
[3] R. Usiskin, J. Maier, Advanced Energy Materials (2020) 2001455.
(Invited) Quantum Dots and Superconductivity in Silicon Systems
Authors: Zwanenburg Floris Arnoud , Sousa de Almeida Antonio 
Published: July 2021

Ge/Si core/shell nanowires are suitable candidates for electrically driven spin qubits, and for the creation of Majorana fermions [1]. In highly tuneable hole quantum dots [2, 3], we observe shell filling of new orbitals and corresponding Pauli spin blockade [4]. In nanowires with superconducting Al leads we create a Josephson junction via proximity-induced superconductivity. A gate-tuneable supercurrent is observed with a maximum of ~60 nA [5]. We identify two different regimes: Cooper pair tunnelling via multiple subbands in the open regime the device [6], while near depletion the supercurrent is carried by single-particle levels of a quantum dot operating in the few-hole regime [5,7,8].
Secondly, we create ambipolar quantum dots in silicon nanoMOSFETs. We investigate the conformity of Al, Ti and Pd nanoscale gates by means of transmission electron microscopy [9]. We define low-disorder electron quantum dots with Pd gates [10], and depletion-mode hole quantum dots in undoped silicon [11]. For the latter we use fixed charge in a SiO2/Al2O3 dielectric stack to induce a 2DHG at the Si/SiO2 interface. The depletion-mode design avoids complex multilayer architectures requiring precision alignment and allows directly adopting best practices already developed for depletion dots in other material systems. Finally, we have realized ambipolar charge sensing: we have fabricated a single-electron transistor next to a single-hole transistor, and tuned both quantum dots to sense charge transitions of the other quantum dot. Using active charge sensing the single-electron transistor can detect the few-charge regime in the hole quantum dot [12].
[1] C. Kloeffel et al., Phys. Rev. B 84, 195314 (2011).
[2] M. Brauns et al., Applied Physics Letters 109, p. 143113 (2016).
[3] F. Froning et al., Applied Physics Letters 113, p. 073102 (2018).
[4] M. Brauns et al., Phys. Rev. B 94, 041441(R) (2016).
[5] J. Ridderbos et al., Advanced Materials, 1802257, (2018).
[6] J. Xiang et al., Nature Nanotechnology 1, 3 (2006).
[7] J. Ridderbos et al., Physical Review Materials, 3, 084803 (2019).
[8] J. Ridderbos et al., Nano Letters 20, 1, p. 122 (2020).
[9] P. C. Spruijtenburg et al., Nanotechnology, (2018).
[10] M. Brauns et al., Scientific Reports 8, 5690, (2018).
[11] S. V. Amitonov et al., Applied Physics Letters 112, p. 023102 (2018).
[12] A. J. Sousa de Almeida et al., Phys. Rev. B 101, 201301(R) (2020).

Figure 1