bluuebunny/crossref_metadata_2025_split huggingface dataset:
Comprehensive Analytical Method with a Standardized Data Pipeline Enables Parallel Experiments in Electrochemical CO2 Reduction
Authors: Senocrate Alessandro , Kraus Peter , Bernasconi Francesco , Battaglia Corsin 
Published: December 2024

The electrochemical reduction of CO2 (eCO2R) is a promising way to convert detrimental CO2 emissions into sustainable fuels and chemicals, and thus to achieve a net zero or net negative carbon economy.
1 Depending on catalyst type and reaction conditions, different gaseous and liquid products can be obtained during eCO2R, with their production rates significantly varying over time. Thus, for any catalytic performance analysis, it is key to assess the product distribution online during eCO2R.
2,3 However, while gaseous products are readily analyzed online by gas chromatography, liquid products are typically only assessed at the end of the reaction due to the lack of suitable automated liquid sampling and analysis methods. In addition, relevant reaction parameters such as CO2 flow rates, electrolyzer temperatures and flow pressures are seldom recorded, causing the loss of important information on catalysts, electrodes, and electrolyzer behavior.
In this work, we overcome these issues by assembling a comprehensive analytical system coupling online gas and liquid product analysis by gas and liquid chromatography (leveraging a special automated liquid sampling valve) with electrochemical protocols that assess CO2RR performance, electrolyzer cell resistance and electrode surface area. In addition, we record CO2 volumetric flow rates, electrolyzer temperatures, as well as gas and liquid flow pressures.
4 To rapidly and reproducibly handle the large and heterogeneous data volume obtained we implement a standardized data pipeline based on our own open-source software,5 which automatically parses the numerous different raw data files, composes a data set following FAIR practices,6 and post-processes and plots the data in a standard way. We validate this analytical system by carrying out eCO2R at 200 mA/cm2 on Cu gas diffusion electrodes, following the changes in selectivity with reaction time for > 12 gaseous and liquid products while recording volumetric flow rates, electrolyzer cell resistance, electrode surface area, electrolyzer temperatures and flow pressures. The modular nature of our analytical system, combined with the standardized data pipeline, allows us to freely increase the number and type of sensors used with minimal impact on the data analysis time, as well as to multiplex our analysis to 8 parallel electrolyzer cells, providing a deep understanding of the function of eCO2R catalysts, electrodes, and electrolyzers, and paving the way to accelerated discoveries.

References

[1] Senocrate, Battaglia, J. Energy Storage
2021, 36, 102373.
[2] Wang, de Araújo, Ju, Bagger, Schmies, Kühl, Rossmeisl, Strasser, Nat.
Nanotechnol.
2019, 14, 1063. [3] Löffler, Khanipour, Kulyk, Mayrhofer, Katsounaros ACS Catal.
202
0, 10, 6735.
[4] Senocrate, Kraus, Bernasconi, Battaglia, Nature Catalysis, accepted.
[5] https://dgbowl.github.io

[5] Kraus, Vetsch, Battaglia, Journal of Open Source Software
2022, 7, 4166.
(Keynote) Electrochemical Conversion of Atmospheric CO2 to Value-Added Products
Authors: Ko Youngdon , Diaz-Abad Sergio , Osmieri Luigi , Zhang Hanguang , Zelenay Piotr 
Published: December 2024

Climate change is an existential threat to humanity that calls for immediate reduction of CO2 concentration in the atmosphere. While drastic reduction in green-house gas emissions needs to remain the primary objective, possible integration of the direct air capture (DAC) and electrocatalytic conversion of CO2 represents a promising strategy to aid in averting a climate catastrophe. In this presentation, we will summarize the recent progress in electrochemical conversion of CO2 to value-added products at Los Alamos, in which we combine experimental and modeling approaches to tackle challenges in the development of materials for the integration of DAC with electrochemical CO2 reduction reaction (CO2RR), mostly concentrating on the conversion part. We use a “5M” (make, measure, model, machine-learn, and modify) approach to accelerate the understanding of how CO2 sorbents and CO2RR catalysts synthesis impacts their structure and performance.
Enhancing electrocatalytic activity and selectivity for the desired products are the main priorities in the development of electrocatalysts for CO2RR.1 Understanding local environment, e.g., local pH and triple phase boundary at the reaction area is also essential for long-term operation of CO2RR devices.2 We will discuss the development of atomically dispersed Ni-N-C catalysts with high selectivity for CO2 conversion to CO (faradaic efficiency in excess of 90%) and the effect that the ionomer used in the electrode preparation has on the Ni-N-C catalyst performance. In particular, we will shed light on how the ionomer properties such as hydrophobicity, local pH, and backbone structure affect the CO2RR activity and selectivity by modifying the ionomer-catalyst interface. In addition, we will outline our approach to facilitating the highly challenging integration of the DAC and CO2RR components via the use of electronically conductive carbon nanofibers with high CO2 sorption capacity and thermo-oxidative resistance.

Acknowledgement

Research presented in this work has been supported by the Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory under project number 20230065DR.

References

(1) Li, Y.; Wang, H.; Yang, X.; O'Carroll, T.; Wu, G. Designing and Engineering Atomically Dispersed Metal Catalysts for CO2 to CO Conversion: From Single to Dual Metal Sites. Angewandte Chemie International Edition
2024, 63 (12), e202317884.
(2) Chen, J.; Wang, L. Effects of the Catalyst Dynamic Changes and Influence of the Reaction Environment on the Performance of Electrochemical CO2 Reduction. Advanced Materials
2022, 34 (25), 2103900.
Increasing the In Vivo Stability of Electrochemical-Aptamer Based Sensors
Authors: Leung Kaylyn , Gerson Julian , Downs Alex , Emmons Nicole , Heemstra Jen , Kippin Tod , Plaxco Kevin 
Published: December 2024

The ability to measure drug, metabolite and biomarker levels in the living body, in real time, and at high frequency would revolutionize our ability to understand and diagnose disease and personalize and guide its treatment. To this end, the Plaxco group has been developing electrochemical aptamer-based (EAB) sensors, a platform technology able to measure molecules in the living body independently of the chemical or enzymatic reactivity of its targets. This has enabled the development of sensors capable of measuring both drugs (e.g., antibiotics, chemotherapeutics, psychoactive substances) and biomarkers (e.g., creatinine, urea, phenylalanine) in live rats.
Though these high time resolution measurements show promise for continuous monitoring, multiple obstacles remain. One example is the challenging environments found in the living body where EAB sensors are deployed can detrimentally affect the longevity of these sensors. As such, I will describe the mechanisms that affect the in vivo lifetime of EAB sensors and methods by which this can be greatly improved.
3-D Mapping Approach for High-Efficiency and High-Precision Latent Flaw Detection
Authors: Yamaura Daichi , Sakata Yoshitaro , Terasaki Nao 
Published: December 2024

In semiconductor manufacturing, fine-polishing process plays important role in achieving high-performance products. In recent years, driven by the escalating demand for process precision, the formation of latent flaws formation, which are defects that cannot be detected by general inspection, during fine-polishing process has emerged as a critical concern. Latent flaws cannot be observed with optical or electron microscopes and require destructive inspection such as etching for reliable detection. Previously, we have reported successful detection of latent flaws by applying stress [1] or heat [2,3] to the substrate.
In this presentation, we present the development of a three-dimensional(3D) mapping approach for detecting latent flaws in glass substrates. Initially, defects were induced in a glass substrate through laser processing (532 nm). Subsequently, by observing the light scattering of the defects while adjusting the focus of the microscope, we analyzed not only the two-dimensional (2D) distribution of latent flaws but also their 3D distribution (Figure), with the addition of depth information. Understanding the depth of latent flaws is crucial, as it provides essential information for calculating the margin for shaving required for repolishing, which is necessary for removing the latent flaws and other defects. Furthermore, the 3D mapping information is anticipated to be valuable not only for optimizing polishing parameters but also for investigating any issues that may arise during the process.
The data obtained from the described methods can be incorporated into a machine learning model to predict the depth of latent flaws from the image data. Our approach enables not only highly sensitive but also highly efficient inspection and is expected to make a significant contribution to the semiconductor manufacturing industry.
[1] Yoshitaro Sakata et al. “Stress-induced light scattering method for the detection of latent flaws on fine polished glass substrates” REVIEW OF SCIENTIFIC INSTRUMENTS 85, 083303 (2014)
[2] Yoshitaro Sakata et al. “Microscopic study of stress effects around micro-crack tips using a non-contact stress-induced light scattering method” AIP ADVANCES 6, 095315 (2016)
[3] Yoshitaro Sakata et al. ” Development of a novel non-contact inspection technique to detect microcracks under the surface of a glass substrate by thermal stress-induced light scattering method” Optics & Laser Technology 90 80–83 (2017)

Figure 1
3D-Printed Molecularly Imprinted Polymers: Advanced Molecular Recognition Interfaces for Chem/Bio Sensors
Authors: Mizaikoff Boris 
Published: December 2024

Molecularly imprinted polymers (MIPs) are known for their stability and specificity serving as biomimetic molecular recognition motif in applications including but not limited to diagnostics, drug delivery, and environmental monitoring. Despite their straightforward synthesis and robustness, the commercial scale-up of MIPs remains challenging, in particular concerning homogeneity and reproducibility of the material and structure, which are both critical for practical applications.
To overcome these challenges, we have developed an innovative strategy synergistically combining LCD-based 3D printing with MIP technology, which enables a yet unprecedented level of manufacturing precision and structural reproducibility. The integration of photo-curing-based 3D-printing with polymerization-induced phase separation constitutes a key advancement facilitating the scalable fabrication of complex macroscopic polymer structures. In addition, the inherent porosity of the material can be precisely controlled at the sub-micrometer level, while at the same time tuning the macro-porosity of the geometric structure via digital design.
This hybridization of techniques marks a new era for MIPs facilitating the production of materials with precison-engineered properties that meet the demanding requirements of a wide variety of applications. Resulting, a robust and scalable approach has been developed that not only improves the reproducibility of MIPs, but also expands their applicability and promises a rapid transition from laboratory innovation to commercial reality. This process is particularly suitable for coating and structuring molecular chem/bio sensing architectures at the surface of electrodes, waveguides and other transducers establishing next-generation biomimetic sensing schemes.

Figure 1
Deep Microfabrication of Silica Glass Using Atmospheric Gas-Phase Catalyst Etching for Sensing Applications
Authors: Sano Kohei , Ono Yoshitaka , Yasuda Kohei , Tobinaga Ryosuke , Imamura Yutaka , Hayashi Yasuo , Yanagitani Takahiko 
Published: December 2024

Deep microfabrication processes such as the Bosch process have dramatically improved the performance of Si-MEMS devices. In contrast to Si, SiO2 is suitable for optical analysis devices because of its high transparency over a wide range and chemical durability. In recent years, micro-total analysis systems using glass-type microfluidics or microwell arrays have attracted attention in the field of biotechnology. Anisotropic microstructures on silica glass substrates are generally fabricated via reactive ion etching (RIE). However, high-power ion energy is required to fabricate deep microstructures because of the high chemical and plasma durability of SiO2. Therefore, the fabrication of vertical deep microstructures on SiO2 has been a longstanding problem because a hard mask material is etched simultaneously during RIE. We focused on surface treatment with HF gas, which enables dry etching of SiO2 without using a plasma source1,2. The chemical reaction between HF gas and SiO2 can be expressed as follows:
SiO2 + 4HF → SiF4 + 2H2O.
However, the etching reaction of SiO2 by HF molecules is extremely slow1. Therefore, H2O or alcohol, which form hydrogen bonds with HF molecules, are added as a catalyst in the etching of SiO2 with HF gas2,3.
This study proposed the deep microfabrication of SiO2 by HF gas etching using a photoresist as a catalyst that allows micro-scale patterning on the substrate4. The hydrophilic functional groups in the catalyst formed hydrogen bonds with the HF molecules at the interface with SiO2. Therefore, the etching reaction by HF gas occurs only at the interface between SiO2 and the catalyst. This selective etching reaction enables deep microfabrication on SiO2 without the use of a plasma source or hard mask materials. The microstructures fabricated via the HF gas-phase catalyst etching were characterized by high verticality and smooth sidewall surfaces, as shown in Fig.1. This simple microfabrication process could improve the sensing performance and the mass production of SiO2-based microfluidic devices and microwells.
REFERENCES

Habuka, H.; Otsuka, T. Reaction of Hydrogen Fluoride Gas at High Temperatures with Silicon Oxide Film and Silicon Surface. J. Appl. Phys., 1998, 37, 6123–6127.

Holmes, P. J.; Snell, J. E. A Vapor Etching Technique for the Photolithography of Silicon Dioxide. Microelectronics and Reliability, 1966, 5, 337–341.

Jang, W. I.; Choi, C.A.; Lee, M.L.; Jun, C.H.; Kim, Y.T. Fabrication of MEMS Devices by Using Anhydrous HF Gas-Phase Etching with Alcoholic Vapor. Micromech. Microeng., 2002, 12, 297–306.

Sano, K.-H.; Ono, Y.; Tobinaga, R.; Imamura, Y.; Hayashi, Y.; Yanagitani, T. (in press). Atmospheric Gas-phase Catalyst Etching of SiO2 for Deep Microfabrication Using HF Gas and Patterned Photoresist. ACS Appl. Mater. Interfaces, Apr. 2024.

Figure 1
(Sensor Division Early Career Award Address) Advancing Hydrogen Technologies with Real-Time Ion Sensing and Tracking
Authors: Dong Dongmei 
Published: December 2024

As we strive for a sustainable future through a green hydrogen economy, it is essential to understand the degradation mechanisms of hydrogen-focused electrochemical devices, such as proton exchange membrane (PEM) fuel cells and water electrolysis systems. Our research delves into current accelerated stress tests and the resulting degradation phenomena through associated comprehensive analyses that include electrochemical, spectroscopic, tomographic, and microscopic techniques, along with detailed examinations of electrode, membrane, and interface structures. Current studies often rely on sophisticated, stationary laboratory equipment to uncover these degradation features under dynamic operations. However, for practical applications like hydrogen-powered electric vehicles, there is a critical need for a portable, low-cost, and user-friendly diagnostic tool.
Given the crucial role of ion exchange and transport, nanoparticles and polymers and the potential for dissolution, monitoring, and tracking ion traces over time can provide critical insights into the behaviors within PEM-based fuel cells and water electrolysis systems. Our recent work focuses on creating electrochemical and transistor-based ion sensors integrated into a circuit chip for real-time, in-situ monitoring of system health and degradation. This effort not only aims to improve real-time diagnostics but also provides guidelines for developing suitable accelerated stress test protocols to assess system durability and for designing materials that can withstand long-term use.
(Digital Presentation) An Integrated Platform for Immune Profiling and Cytokine Monitoring
Authors: Kang Xuejia , Zhou Lang , Ma Chao , Wang Chuanyu , Wu Shuai , Wu Siqi , Chen Weiqiang , Rampauram Jayachandra Babu , Chen Pengyu 
Published: December 2024

In the realm of cancer immunotherapy, the pivotal role of immune cells in driving efficacy, and the delicate balance maintained by cytokines between efficacy and potentially life-threatening side effects, cannot be overstated. Hence, precise in situ immune profiling and close scrutiny of critical cytokines are imperative for assessing the features associated with immunotherapeutic interventions. Unfortunately, existing in vitro assessment methods suffer from drawbacks such as being endpoint, time-intensive, and demanding large sample volumes.
To address these limitations, we present an innovative solution: an integrated real-time 3D vascularized blood-brain barrier (BBB) chip. This cutting-edge platform faithfully replicates the BBB environment infiltrated by immune T cells while simultaneously enabling the monitoring of immune profiling. Crucially, it facilitates the real-time detection of cytokines during CAR T cell interactions with various cell types. This comprehensive monitoring encompasses crucial aspects such as T cell and monocyte migration, cancer cell recognition, immune cell activation, and cytokine and neurotransmitter dynamics. Furthermore, the chip allows for the evaluation of the dynamics of therapeutics aimed at managing side effects associated with immunotherapy.
A key highlight of our approach is the ability to detect cytokines directly within the biological milieu. This method exhibits an impressive detection range spanning from 1 to 10,000 pg/mL, requiring only a minimal sample volume of 4 μL. The innovative sensing mechanism utilizes pillar microarrays, where anti-cytokine capture antibodies (CAbs) immobilized as the primary layer efficiently capture cytokines. Paired detection antibodies (DAbs) then facilitate signal detection, enabling simultaneous detection of multiple cytokines within small sample sizes through parallel processing.
By providing a means to effectively monitor the dynamics of immune therapy-induced factor release without perturbing the cancer microenvironment, our integrated chip empowers researchers to delve deeper into the intricacies of immunotherapy while enhancing its safety profile. This advancement holds significant promise for improving the outcomes of cancer treatment, ushering in a new era of precision and efficacy in cancer immunotherapy.
Effect of Direct Current and Periodic Polarization on Differential Electrolytic Potentiometric Signal Produced By Carbon Nanotube Electrode
Authors: Osman Abdalghaffar Mohammad 
Published: December 2024

In differential electrolytic potentiometry (DEP), a pair of identical indicator electrodes is polarized using either a very small, heavily stabilized direct current (DC) or a periodic square waveform (SW) of constant amplitude. The square wave can be biased or bias-free. In this study, carbon nanotube-modified silver electrodes, CNT-Ag, were used as the DEP indicating system with all types of polarization. This was done to investigate how the polarization mode affects the signal intensity, shape, position, and amplification. The method was applied to analyze various analytes including ascorbic acid, Fluoroquinolone, cyanide, and chloride using normal titrimetric and sequential injection analysis (SIA) methods. Many of the findings showed that raising the polarizing direct current density (µA/cm2) boosts the DEP peak until reaching a certain point, after which the peaks begin to widen and the position of the peak center shifts. Similar changes were observed when increasing the percentage bias of the square waveform used to polarize the CNT-Ag indicator electrodes. The free-biased square waveform led to the least improvement in peak intensity. As the percentage bias increased, the peak intensity improved up to a certain level. However, beyond that point, all peaks began to broaden without further enhancement in intensity. In all cases, periodic polarization of electrodes produced a much greater enhancement in peak intensities compared to direct current polarization. With square-wave polarization, the ongoing reversal of polarity prevents the accumulation of films on the electrodes, speeds up the response, and substantially reduces electrode fouling and deactivation.
Furthermore, aside from the advantages of the periodic polarization, the CNT-Ag electrode, fabricated through chemical vapor deposition with aligned and well-structured CNTs, contributes to boosting the DEP peak intensity by promoting heterogeneous electron transfer. This process facilitates fast equilibrium, leading to precise and reproducible results.

Figure 1
Bay-Region, Nitrogen Functionalized Perylene Diimides for Printed Electronic Sensors
Authors: Welch Gregory Charles 
Published: December 2024

The chemistry of organic conjugated materials is rich. Chemical structures can be infinity tuned to tailor optical, electronic, and physical properties. With an ability to transport electrical charge, such materials have found widespread use in electronic devices ranging from solar cells to sensors, so called ‘organic electronics. As organic electronic technologies move towards commercialization there becomes a focus on cost and sustainably. Perylene diimide (PDI) is a classic organic dye that has been well manipulated and studied in organic electronics and championed as chemically versatile, high-performance, and accessible (i.e. low-cost). While many electronic devices featuring PDI as an active electronic component have been engineered to achieved high performance, sustainably (i.e. greenness) has often been overlooked. Our research team at the university of Calgary is a member of the Canadian NSERC Green Electronics Network (GreEN) developing new materials and processes for sustainable organic electronic devices. This presentation will showcase two new PDI dyes, modified with active pyrrole or amine functional groups to produce electronically active, large area, green solvent roll-coated films. The materials design, chemistry, properties, and utility as electronic amine sensors, fully roll coated, will be discussed.
References:

Flexible dual-action colorimetric-electronic amine sensors based on N-annulated perylene diimide dyes. RSC Sensors and Diagnostics. Early View. 10.1039/D4SD00004H

Organic heterojunction charge-transfer chemical sensors. Journal of Materials Chemistry C. 2024. 12, 5083-5087.

An air-stable n-type bay-and-headland substituted bis-cyano N-H functionalized perylene diimide for printed electronics. Journal of Materials Chemistry C. 2021. 9, 13630-13634.

Acid dyeing for green solvent processing of solvent resistant semiconducting organic thin films. Materials Horizons. 2020. 7, 2959-2969.