bluuebunny/crossref_metadata_2025_split huggingface dataset:
Is It Greener? Impact of Cathode Catalyst Performance on Life-Cycle Emissions of Producing Methanol By Electrocatalytic CO2 Reduction
Authors: Pellow Matthew , Benson Sally 
Published: February 2020

Direct electrocatalytic reduction of carbon dioxide (deCO2rr) is being developed as a route to energy-dense liquid transportation fuels for a low-emissions future. This technology would reduce net emissions from fuel combustion, because these would be fully offset by upstream capture of the CO2 used to produce the fuel. However, it would produce some additional emissions from related processes, such as generating the process electricity and purifying the product stream. Although extensive basic-science catalysis research is underway in this area, the full life-cycle emissions of this technology platform have not been quantified.
In this prospective technology analysis, we apply systematic life cycle assessment (LCA) to estimate the total life cycle emissions associated with producing methanol from low-temperature electrocatalytic reduction of CO2. This analysis framework (1) quantifies the emissions impact of using deCO2rr to provide drop-in liquid hydrocarbon fuels, and (2) provides catalyst performance targets (faradic efficiency, overpotential, and yield) for this technology to provide net emissions reductions. The framework provides a long-term emissions impact perspective to guide priorities in catalysis research for sustainability.
The hypothetical reference case deCO2rr system in this analysis features a cathode electrocatalyst that reduces CO2 to methanol with 15% faradaic efficiency, 0.8 V overpotential, and 25% conversion of CO2 to product. Water is oxidized at the anode. The methanol production system is coupled to CO2 capture from a coal-fired power plant. In a preliminary analysis of this integrated methanol-electricity system, the products (1 g MeOH plus 6.1 Wh of electricity) have a total emissions intensity of 3.8 g CO2. This is approximately half the emissions produced when using conventional processes to produce the same electricity (without carbon capture) and methanol (using a natural gas-based process).
In addition, we quantify the emissions impact of improving the performance of the CO2 reduction catalyst from present values. We identify technology performance thresholds for this renewable methanol process to provide a net emissions reduction compared to conventional processes. For instance, we estimate that using present-day CO2 capture technology, the integrated electricity-methanol production system would provide a net reduction in emissions if the cathode catalyst has 20% faradaic efficiency and 20% molar conversion of CO2 to methanol.
Catalytic Activities of Sulfur Atoms in Amorphous Molybdenum Sulfide (MoSx) for the Electrochemical Hydrogen Evolution Reaction
Authors: Yeo Boon Siang 
Published: February 2020

In-situ Raman spectroscopy during cyclic voltammetry was used for the first time to investigate the hydrogen evolution reaction (HER) occurring on electrodeposited amorphous MoSx films, which consist of Mo3-based motiffs. A Raman peak at 2530 cm-1 was observed on these films during HER in aqueous HClO4 electrolyte. This peak was assigned as a MoS-H stretching vibration. This identification was corroborated by H/D isotopic exchange experiments. Hence, we could directly establish that sulfur atoms are the catalytic active sites in amorphous MoSx for proton reduction.
We further distinguish the activities of the S atoms present in these amorphous films. Using X-ray photoelectron spectroscopy as a means to identity the types of S atoms present, we found that the turnover frequency for H2 production increases linearly with the percentage of S atoms with higher electron binding energies. These S atoms could be apical S2- and/or bridging S2
2-. Quantum chemical simulations using density functional theory rule out the apical S2- atoms as reaction sites for HER. In situ Raman spectroscopy of the model [Mo3S13]2- cluster further demonstrate the higher catalytic reactivity of the bridging S2
2- over terminal S2
2- (which have lower electron binding energy) for proton reduction.
Hierarchically Structured Zinc Oxide Gas Sensors with Silver Catalyst
Authors: Chung Yoonsung , Park Hyejin , Lee Eunji , Kim Dong-Joo 
Published: February 2020

During the last few years, interest in wearable devices including a portable and wearable gas sensor system has increased. Since integration of fabric and gas sensors for a wearable breath monitoring system would allow continuous monitoring patients’ breathing gases such as acetone gas for diabetes (1), ammonia for renal disease (2), and ethanol for hepatic steatosis (3), realization of a miniaturized wearable gas sensor operating at daily environment is in demand.
Zinc oxide has definite advantages over other semiconducting nano-scale metal oxides because of its electric properties such as wide bandgap and high electron mobility (4). ZnO nanostructures have been investigated such as nanorods, nanotubes, and nanowires. Recently, hollow micro/nanosphere ZnO has been attracting attention. It may be able to apply for dye-sensitized solar cells, photocatalts, high performance electrodes, and gas sensors due to its large surface-to-volume ratio and reduced transport lengths for both mass and charge transport (5).
The researches about the catalytic decoration of ZnO gas sensors by metallic nanoparticles or layers have been also investigated to improve selectivity (6, 7). Especially, ZnO with silver is considered to exhibit relatively high sensitivity to ethanol (7).
In this study, the hollow microsphere ZnO particles were prepared by a simple but new precipitation method and then Ag sputter coated. Electrophoretic deposition (EPD) of the hollow particles with Ag was then used to construct ZnO-Ag layers on flexible polyimide films. The structural properties of the deposited ZnO layers were analyzed by using SEM, TEM, and XRD. Then, gas sensing behaviors to detect ethanol, acetone, and ammonia by thickness of Ag are discussed in detail.
This research was partially supported by the Korea Institute of Energy Technology Evaluation and Planning (20158520000210) grant funded by the Korea Government Ministry of Trade, Industry and Energy, a grant from a Strategic Research Project (2013-0132) funded by the Korea Institute of Construction Technology, and Auburn University IGP.
(1) Zhang, Q., Wang, P., Li, J., and Gao, X. (2000) Biosens. Bioelectron.
15, 249-256
(2) Moorhead, K. T., Lee, D., Chase, J. G., Moot, A., Ledingham, K., Scotter, J., Allardyce, R., Senthilmohan, S., and Endre, Z. (2008) Computer methods and programs in biomedicine
89, 226-238
(3) de Lacy Costello, B., Ewen, R., Ratcliffe, N. M., and Richards, M. (2008) J. Breath Res.
2, 037017
(4) Ahn, H., Park, J.-H., Kim, S.-B., Jee, S. H., Yoon, Y. S., and Kim, D.-J. (2010) Electrochemical and Solid-State Letters
13, J125-J128
(5) Xie, Q., Li, J., Tian, Q., and Shi, R. (2012) Journal of Materials Chemistry 22, 13541-13547
(6) Lupan, O., Chow, L., Ono, L. K. Ono, Cuenya, B. R., Chai, G., Khallaf, H., Park, S., and Schulte, A. (2010) The Journal of Physical Chemistry C
114, 12401-12408
(7) Lyashkov, A. Yu, Tonkoshkur, A. S., Aguilar-Martinez, J. A. and Glot, A. B. (2013) Ceramics International
39, 2323-2330
Real-Time Monitoring of Superoxide Anion Radical and Hydrogen Peroxide Generation in Higher Plants in Response to Wounding: In-Vivo Electrochemical Study
Authors: Prasad A. , Takahashi A. , Fujii R. , Matsuoka R. , Kikuchi H. , Aoyagi S. , Aikawa T. , Kondo T. , Yuasa M. , Tada M. , Kobayashi M. , Pospíšil P. , Kasai S. 
Published: February 2020

The growth and development in plants are deleteriously affected by various biotic and abiotic stress factors. Wounding in plants occurs with exposure to environmental mechanical stresses or via herbivory. The response of plants towards wounding have been categorized based on the response time; the fast response includes oxidative burst accompanied by generation of reactive oxygen species (ROS) or delayed response which includes transcriptional activation of wound-induced genes, deposition of callose, accumulation of proteinase inhibitors and hydrolytic enzymes etc. The oxidative burst in response to wounding is known to be associated with the formation of various ROS such superoxide anion radical (O2
•−), singlet oxygen and hydrogen peroxide (H2O2). In the current study, we provide experimental evidences and real time monitoring of O2
•−
and H2O2 generation following wounding in leaves of spinach (Spinacia oleracea).
Real-time monitoring of ROS generation was achieved using amperometric method utilizing different electrodes. Non-specific real-time measurements of ROS were done by monitoring the changes in reduction current using carbon electrode while qualitative and quantitative measurement of O2
•−
and H2O2 generationwere done using newly developed iron-porphyrin based modified carbon electrodes and osmium-horseradish peroxidase (Os-HRP) based modified carbon electrodes, respectively. The results obtained showed continuous generation of O2
•− and H2O2 for minutes after injury followed by a decline. The activation of lipoxygenase after wounding; its involvements in the production of H2O2 and the contribution of H2O2 in generation of local response in injured plant tissue besides the initiation of systemic response caused by hormones such as jasmonic acid, ethylene, salicylic acid, and abscisic acid will be disscussed.
Detection of Cortisol in Pbs Buffer and Fish Blood Plasma By Electrochemical Impedance Spectroscopy
Authors: Pali Madhavi L , Suni Ian Ivar 
Published: February 2020

Cortisol (MW = 362.5) is a steroid hormone produced in the human body by the adrenal gland in response to elevated levels of stress. Normal levels of cortisol in the human body range from 6-23 microgram per deciliter. Cortisol has also been widely studied in order to better understand fish physiology, with applications to fish ecology and fish farming, since cortisol levels can also be employed as a biomarker for reproductive activity.
Following immobilization of the polyclonal antibody to cortisol atop an Au electrode, we have detected cortisol in both PBS buffer solution and fish blood plasma, with a detection range up to 0.5 microgram/ml. Binding of cortisol approximately follows the Langmuir adsorption isotherm, and the detection range is limited at high concentrations by saturation of the antibody film. This allows the use of sample dilution to reduce the physiological concentration of cortisol down to the range in which it can be detected by impedance biosensing. The advantage of this approach is that non-specific adsorption is also dramatically reduced by sample dilution. Non-specific adsorption in this system is unmeasurable, due to both the use of sample dilution and the use of BSA for surface blocking.
(Invited) Recent Density Functional Theory Investigations in Electrode Materials for Rechargeable Batteries
Authors: Arroyo-de Dompablo Elena 
Published: February 2020

First-principles computation is recognized as an invaluable tool in designing new electrode materials for lithium ion batteries (LIBs). Numerous achievements in predicting relevant properties (including voltage, structure stability, electronic property and ionic mobility) of electrode materials for LIBs using Density Functional Theory has been reported in the last two decades (see, for instance, reference 1). Beyond the LIB technology, computational tools are critically important to enable the development of alternative energy storage technologies. In the last years, concerns on Li availability have prompted the search for suitable alternatives to rechargeable LIBs. Batteries based on multivalent charge carriers (Mn+) can exhibit advantages in terms of energy density since for a certain amount of M carriers the capacity is doubled (n=2) or tripled (n=3) when compared to single valent carriers like Li+ or Na+. Calcium is an attractive candidate due to its low cost, natural abundance and low reduction potential. The feasibility and reversibility of calcium plating in conventional alkyl carbonate electrolytes at moderate temperatures has been recently reported [2]. Such finding opens the way to the development of a new rechargeable battery technology using calcium anodes. The identification of potential cathode and anode materials is a must to open the research avenues for the new calcium based battery technology (CIBs). In this contribution, we will show recent progress in first principles computation in predicting, understanding and improving the electrochemical properties of selected electrode materials for Li, Na, Mg and Ca ion batteries.
Acknowledgments: The author thanks P. Tartaj (LIBs), F. Bardé (CIBs) and M.R. Palacin for the experimental work. Financial support from Ministerio de Ciencia e Innovación (grant MAT-2011-24757) and Toyota Battery Research division at Higashi Fuji (M6) is acknowledged.
[1] Y.S. Meng and M.E. Arroyo-de Dompablo, Energy and Environ. Science 2, 589, 2009
[2] A. Ponrouch, C. Frontera, F. Barde, M. R. Palacin. Nature Materials, DOI:10.1038/NMAT4461
Multiscale Computational Approaches for the Simulation of Battery Electrodes Fabrication
Authors: Franco Alejandro A. , Shukla Garima , Morcrette Mathieu , Cavalaglio Sebastien 
Published: February 2020

The automotive lithium ion battery (LIB) industry has reached a point where optimization studies are vital to achieve high performance at low environmental and economic cost. Significant progress has been made in linking structural properties to ionic transport and cell capacity response using either computer-aided reconstruction of real electrode structure or modeling on built artificial structures [1-2]. However a more holistic approach by combining electrode composition with fabrication parameters is crucial to produce results coherent with experiment. Computational modeling constitutes a powerful tool to establish such an approach, but until now only very few theoretical efforts on this topic have been reported so far [3-4].
In this contribution we aim to mimic standard LIB electrode fabrication techniques through innovative multiscale modelling and numerical simulation [5]. With electrode composition as a control parameter [4,6], respective interactions at the mesoscale level between the active material, conductive material, solvent, binders and dispersants are being considered within an in house three-dimensional Monte Carlo (MC) simulation approach describing the slurry preparation and the solvent evaporation (Figure). The simulations provide insights into the self-organization mechanisms of materials during fabrication as function of the composition, particles size distribution and polymer binder lenght. More specifically, we discuss here the efficiency, advantages and disavantages of using two types of MC methods, namely Metropolis MC and Kinetic MC through the Variables Step Size Method [7-8], on predicting the pore size distributions, porosity and effective electronic conductivity of LIB electrodes.
The potential of these simulations to lead to proposals of new and highly efficient fabrication techniques is discussed in view of the wide diversity of active material chemistries now emerging for LIB applications.
[1] A. A. Franco, RSC Adv., 3(2013) 13027.
[2] Stephen E. Trask, Yan Li, Joseph J. Kubal, Martin Bettge, Bryant J. Polzin, Ye Zhu, Andrew N. Jansen, Daniel P. Abraham, J. Power Sources, 259(2014) 233.
[3] Z. Liu, P.P. Mukherjee, Journal of The Electrochemical Society, 161
(8) (2014) E3248.
[4] Z. Liu, V. Battaglia, P.P. Mukherjee, Langmuir, 30
(50) (2014) 15102.
[5] Physical Multiscale Modeling and Numerical Simulation of Electrochemical Devices for Energy Conversion and Storage: From Theory to Engineering to Practice. A.A. Franco, M.L. Doublet, W.G. Bessler (Eds.), Springer (2015).
[6] G. Liu, H. Zheng, X. Song, V. S. Battaglia J. Electrochem Soc., 159(3) (2012) A214.
[7] M.A. Quiroga, A.A. Franco, J. Electrochem. Soc., 162 (7) (2015) E73.
[8] G. Blanquer, Y. Yin, M.A. Quiroga, A.A. Franco, J. Electrochem. Soc., 163 (3) (2016) A329.

Figure 1
Image-Based Reconstruction and Statistical Characterization of Li-Ion Battery Electrode Microstructures
Authors: Mukherjee Rajib , Mistry Aashutosh , Mukherjee Partha P. 
Published: February 2020

Lithium-ion battery electrodes are composite structures that contain multiple phases including electroactive material, conductive additive and polymer binder. The stochastic microstructure thus formed consists of particulate materials and pore network. The pore scale characteristics of the electrode determine the properties of battery. An accurate estimation of microstructural characteristics is essential for structure property relation that will enable use to design and develop batteries with enhanced properties. With the advancement in X-ray micro-/nano-tomography, details of the electrode microstructure can be probed. Tomographic images of porous electrode microstructures can be obtained at various depths or from different angles. The stack of images needs to be processed for accurate segmentation of pore and particle distribution in the matrix for statistically significant microstructure reconstruction. In the present work, image-based reconstruction of Li-ion battery electrode microstructures and subsequent statistical and transport characterization is presented. In image-based microstructure reconstruction, the segmentation is a critical step that determines the transport networks in the porous matrix. Various algorithms can be employed for segmentation including watershed transform, region merging, graph partitioning. Segmentation methods can be manual, computer assisted or hybrid. In this work, a novel segmentation algorithm has been developed based on region merging method. The segmentation parameter is determined by the fractal nature of the segments, which in the present case is the pore and active particle interface. This enables the segmentation process to be more accurate and automated. The reconstructed electrode microstructures are characterized by its fractal dimension, which is further linked to the transport properties.
Modeling Battery Performance Due to Intercalation Driven Volume Change in Porous Electrodes
Authors: Garrick Taylor Reed , Dai Yiling , Higa Kenneth , Srinivasan Venkat , Weidner John W. 
Published: February 2020

In order to accurately predict the behavior of electrochemical devices, it is necessary to develop sophisticated models that take into consideration transport processes, electrochemical phenomena, mechanical stresses, and structural deformations (i.e. strain) on the operation of an electrochemical system. There are many different models in use that can predict the electrochemical performance of these devices under a variety of operating and design conditions. However, many of these models assume a constant porosity and do not take into consideration the effects of a variable porosity on the porous electrode during cycling and what effects that may have on performance. In recent years, electrodes have been developed that show significant volume changes during intercalation and deintercalation, which are unable to be accurately predicted using these constant porosity models.
Here, a mathematical battery model is presented that incorporates the dimensional and porosity changes in porous electrodes caused by volume changes in the active material during intercalation (e.g., lithium into carbon or silicon). Porosity and dimensional changes in an electrode can significantly affect the resistance of the battery during cycling. In addition, volume changes generate stresses in the electrode, which can lead to premature failure of the battery. Here, material conservation equations were coupled with the mechanical properties of porous electrodes to link dimensional and porosity changes to stresses and the resulting resistances that occur during the intercalation process. The stress-strain relationships used in this model are from previous works, which are used to predict porosity and dimensional changes, and were established by comparing thermal rock expansion and electrode expansion due to intercalation. Several different cases modeled after new battery electrode technologies are examined and operating curves are predicted based off of standard equilibrium potentials.
3D Simulation on the Internal Distributed Properties of Lithium-Ionbattery with Planar Tabbed Configuration
Authors: Cheng Yun , Li Jie , Jia Ming , Du Shuanglong 
Published: February 2020

Lithium-ion batteries have promoted the rapid developments of hybrid and electric vehicles due to their high energy, power density, and long lifetime [1]. Meanwhile, advanced hybrid and electric vehicles accelerate lithium-ion cells to be large sized [2].With the increase of battery cell size, the inhomogeneity of battery also increases, which exists not only between the batteries, but also inside a single battery. The inhomogeneity between batteries mainly refers to the difference in the battery pack. The main indicators are inconsistent battery voltage, internal resistance, capacity, and state of charge [3]. This inhomogeneity will lead certain cells to be the state of long-term over-charged or over-discharged, thus not only shortening the battery life, but also even leading to the combustion or explosion of batteries. The inhomogeneity inside a single battery mainly refers to the non-uniform distribution of the electrochemical reaction rate, current density, active material utilization ratio, and the electrolyte concentration in the electrode plate. The main damage of this inhomogeneity is the inhomogeneity of physicochemical properties such as stress gradient on the electrode plate [4]. In long cycling process, large gradient may lead to high diffusion induced stress (DIS), cause particle fracture and reduce battery capacity [5]. The inhomogeneity between batteries can be reduced or eliminated by the automatic production of battery and equalization module of battery management system (BMS). However, the inhomogeneity inside a single battery is difficult to be characterized or measured because of the sealed battery packaging.
In this paper, a validated three-dimensional (3D) model on the electrode plate level of a lithium-ion battery was developed for a commercial type LP12100115 prismatic power LiFePO4/graphite battery (10 Ah) by coupling mass, charge, and energy conservations, as well as electrochemical kinetics. This model can intuitively show the space and time distribution characteristics of the internal electrochemical properties of the lithium-ion battery such as the transient distribution of electric potential, over-potential, state of charge, current density and lithium-ion concentration. The extraction of these distribution characteristics can significantly affect the design and optimization of large lithium-ion batteries.
References
[1] B. Scrosati, J. Garche, J. Power Sources. 2010, 195, 2419-2430.
[2] L. Lu, X. Han, J. Li, J. Hua, M. Ouyang, J. Power Sources. 2013, 226, 272-288.
[3] E. Gallardo-Lozano, M.I. Romero-Cadaval, M.A. Milanes-Montero, J. Guerrero- Martinez, Power Sources. 2014, 246, 934-949.
[4] S. Renganathan, G. Sikha, S. Santhanagopalan, R.E. White, J. Electrochem. Soc.
2010, 157, A155-A163.
[5] C. Lim, B. Yan, L. Yin, L. Zhu, Electrochimica Acta. 2012, 75, 279-287.

Figure 1