Colorimetric sensors with instant visual readout are significant and highly required for convenient detection of various analytes, especially in the post-COVID-19 era. Noble metal-based bimetallic nanoparticles (NMBNPs), considered as promising nanoprobes for colorimetric sensing, are significantly superior to monometallic nanoparticles due to their improved optical property, catalytic activity, stability and selectivity. In this review, we focus on the recent progress in the colorimetric sensors based on NMBNPs with alloy, core-shell, core-satellite and Janus nanostructures. Firstly, we comprehensively introduce the synthesis approaches of NMBNPs which can be classified into three classes, including the top-down physical methods, bottom-up chemical methods and other emerging methods. Depending on these NMBNPs, the main sensing strategies exploiting their unique localized surface plasmon resonance (LSPR) property and nanozyme activity for various applications in colorimetric detection are critically summarized and discussed in detail. Finally, challenges and opportunities for the future development of NMBNPs-based colorimetric sensors are proposed and summarized. We hope that this review will help readers to better understand the current research status of NMBNPs for colorimetric sensing. 

Recent development of noble metal-based bimetallic nanoparticles for colorimetric sensing

Electrochemistry-driven techniques for advanced energy storage/conversion and environmental protection play a crucial role in achieving sustainable development goals. As an indispensable component in diverse electrochemical systems, electroactive materials gain soaring interest in terms of rational design and sustainable synthesis. Notably, mechanochemistry-based green and powerful synthesis has been widely employed to fabricate diverse electroactive materials, given their scalability and tunability. Recently, mechanochemically synthesized electroactive materials have been widely applied in various environmental and energy fields, leading to significant progress. However, a systematic analysis of these advancements is still missing. Herein, we comprehensively discuss recent achievements in mechanosynthesized electroactive materials for sustainable energy and environmental applications. The development of mechanochemical synthesis is introduced, along with different types of mechanosynthesized electroactive materials. Subsequently, the review delves into the applications of these materials in advanced energy conversion/storage systems and environmental remediation. The rational design of electroactive materials and their structure-performance correlation are illustrated by discussing the effects of the mechanochemical process on the internal and external properties of materials and their electrochemical performance. Lastly, key perspectives in this field are discussed, including mechanochemical process monitoring, field-assisted mechanochemical synthesis, material performance optimization, practical applications, and mechanochemistry-driven fuels/chemicals synthesis. By illustrating current advances and perspectives related to the development of mechanosynthesized electroactive materials, this review aims to shed some light on upcoming research on green mechanochemical synthesis-driven energy and environmental sustainability. 

Mechanosynthesized electroactive materials for sustainable energy and environmental applications: A critical review

ADVERTISEMENT RETURN TO ARTICLES ASAPPREVReviewNEXTRecent Developments in Single-Entity ElectrochemistryL. ZhangL. ZhangDepartment of Chemistry, Texas A&M University, College Station, Texas 77845, United StatesMore by L. ZhangView Biography, O. J. WahabO. J. WahabDepartment of Chemistry, Texas A&M University, College Station, Texas 77845, United StatesMore by O. J. WahabView Biographyhttps://orcid.org/0000-0003-4280-9089, A. A. JallowA. A. JallowDepartment of Chemistry, Texas A&M University, College Station, Texas 77845, United StatesMore by A. A. JallowView Biographyhttps://orcid.org/0000-0003-2173-4137, Z. J. O'DellZ. J. O'DellDepartment of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United StatesMore by Z. J. O'DellView Biographyhttps://orcid.org/0000-0002-7779-596X, T. PungsrisaiT. PungsrisaiDepartment of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United StatesMore by T. PungsrisaiView Biography, S. SridharS. SridharDepartment of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United StatesMore by S. SridharView Biographyhttps://orcid.org/0000-0003-3379-1630, K. L. VernonK. L. VernonDepartment of Chemistry, Texas A&M University, College Station, Texas 77845, United StatesMore by K. L. VernonView Biography, K. A. Willets*K. A. WilletsDepartment of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States*Email: [email protected]More by K. A. WilletsView Biographyhttps://orcid.org/0000-0002-1417-4656, and L. A. Baker*L. A. BakerDepartment of Chemistry, Texas A&M University, College Station, Texas 77845, United States*Email: [email protected]More by L. A. BakerView Biographyhttps://orcid.org/0000-0001-5127-507XCite this: Anal. Chem. 2024, XXXX, XXX, XXX-XXXPublication Date (Web):May 10, 2024Publication History Published online10 May 2024https://doi.org/10.1021/acs.analchem.4c01406© 2024 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0. License Summary*You are free to share (copy and redistribute) this article in any medium or format and to adapt (remix, transform, and build upon) the material for any purpose, even commercially within the parameters below:Creative Commons (CC): This is a Creative Commons license.Attribution (BY): Credit must be given to the creator.View full license*DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. This publication is Open Access under the license indicated. Learn MoreArticle Views-Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail PDF (7 MB) Get e-AlertscloseSUBJECTS:Collisions,Electrodes,Metal nanoparticles,Nanoparticles,Nanopores Get e-Alerts 

Recent Developments in Single-Entity Electrochemistry.

The electronic conductivity and durability of porous carbon supports can be improved by increasing the degree of graphitization in the material; however, the preparation of highly graphitic porous carbon using conventional furnaces remains a significant challenge. Herein, we demonstrate a universal and highly efficient carbothermal shock strategy that significantly improves the degree of graphitization of porous carbon supports, including bowl-like carbon, hollow carbon spheres, ZIF8-derived carbon, BP2000, and Ketjen EC 300J. Taking bowl-like carbon as an example, we illustrate the synthesis of a graphitized bowl-like carbon (G-BC-S) support and evaluate the performance of PtCo/G-BC-S in the oxygen reduction reaction (ORR) in rotating disk electrodes (RDE) and H2/air PEM single cells. PtCo/G-BC-S exhibits faster ORR kinetics than PtCo/BC and Pt/C, with little loss of activity (25%) and only 13 mV of E1/2 decay after 20000 cycles accelerated stress testing under 1.0–1.5 V vs. a reversible hydrogen electrode (RHE).</a> The significantly enhanced performance of the PtCo/G-BC-S catalyst arises from the high activity and chemical/structural stability of the PtCo intermetallic nanoparticles and from the high degree of graphitization and well-defined porous structure of the bowl-like carbon support, which confers excellent electrical conductivity and oxygen transport properties. This study provides a reliable and universal strategy for the development of high-performance porous carbon supports for practical applications in fuel cells. 

Ultrafast carbothermal shock strategy enabled highly graphitic porous carbon supports for fuel cells

The electroreduction of nitrate offers a promising, sustainable, and decentralized route to generate valuable ammonia. However, a key challenge in the nitrate reduction reaction is the energy efficiency of the reaction, which requires both a high ammonia yield rate and a high Faradaic efficiency of ammonia at a low working potential (≥-0.2 V versus reversible hydrogen electrode). We propose a bimetallic Co-B/Ru 

In-situ electrochemical reconstruction and modulation of adsorbed hydrogen coverage in cobalt/ruthenium-based catalyst boost electroreduction of nitrate to ammonia

Proton-exchange membrane fuel cells (PEMFCs) represent an essential technology for the future decarbonization of the transportation sector. A major component of PEMFCs is the catalyst, often Pt-based alloys supported on carbon black, which are sufficiently active and stable upon long-term operation under the harsh reaction conditions implied by PEMFCs. However, the catalyst synthesis is typically laborious and challenging to upscale, employing organic solvents, surfactants, or uneconomical metal deposition routes. To solve this, we offer a mechanochemically assisted two-step solvent-less methodology to produce supported metal catalysts, particularly supported PtNi and PtCo catalysts. Accordingly, metal salts are first dispersed on the designated support by planetary ball milling. Subsequently, the mixture is reduced with hydrogen and annealed under an inert atmosphere to yield supported alloyed nanoparticles. Notably, by applying our procedure to the synthesis of carbon-supported PtNi and PtCo nanoparticles, we demonstrate that size, composition, and total metal loading can be finely adjusted, leading to highly performant catalysts in the oxygen reduction reaction (ORR). 

Facile Solid-State Synthesis of Supported PtNi and PtCo Bimetallic Nanoparticles for the Oxygen Reduction Reaction

Increasing the resistance of catalysts against electroche-mical degradation is one of the key requirements for the wider use of Proton Exchange Membrane Fuel Cells (PEMFCs). Here, we study the degradation of one entity of a highly stable catalyst, Pt@HGS, on a nanoelectrode under accelerated mass transport conditions. We find that the catalyst degrades more rapidly than expected based on previous ensemble measurements. Corroborated by identical location transmission electron microscopy and catalyst layer experiments, we deduce that locally different pH values are likely the reason for this difference in stability. Ultimately, this work provides insights into the actual conditions present in a PEMFC and raises questions about the applicability of accelerated stress tests usually performed to evaluate catalyst stability, particularly when they are performed in half-cell setups under inert gas.

Stability Investigations on a Pt@HGS Catalyst as a Model Material for Fuel Cell Applications: The Role of the Local pH.

Influence of Support Material on the Structural Evolution of Copper during Electrochemical CO
 2
 Reduction

Cross-sections of morphology-controlled catalysts mixed with ionomer are analyzed with energy-dispersive X-ray spectroscopy. The elemental mappings provide information about the behavior of the ionomer on the nanoscale, including the penetration depth of the ionomer into small mesopores. Furthermore, the suitability of metal ion exchange for tracking the ionomer distribution is validated by post-impregnation with cesium. Ultimately, this work lays the foundation for a meaningful characterization of the ionomer distribution in catalyst layers of proton exchange membrane fuel cells.
 
 
 
 


Insights into the Ionomer Distribution through Elemental Mapping of Model Catalysts Mixed with Nafion

To reach its climate neutrality goal by 2050, the European Union has agreed on ceasing the sale of new petrol and diesel-driven vehicles by the end of 2035. Therefore, interest in carbon-neutral transport options, such as battery-electric vehicles (BEV) or fuel-cell-electric vehicles (FCEV) has tremendously increased. Especially for heavy-duty applications, proton exchange membrane fuel cells (PEMFCs) can be a viable solution, as they exhibit a higher gravimetric power density compared to BEVs.[1] However, cost and supply constraints of the catalyst active material, i.e. platinum, are still a major hurdle to make PEMFCs competitive with incumbent technologies. While this has been addressed by a reduction of the Pt loading, this induces some major drawbacks regarding the overall performance due to the decrease in catalyst activity towards the oxygen reduction reaction (ORR) and the increase in proton and oxygen mass transport resistances to the Pt surface.[2] It has been shown that those issues can be mitigated by using cathode catalyst materials with a mesoporous carbon support, as they exhibit a high ORR activity while additionally facilitating the transport of protons and gaseous oxygen to Pt nanoparticles that are located inside the pores of the carbon support particles.[3] Previous studies have demonstrated that by using a multi-step catalyst synthesis procedure where Pt nanoparticles are incorporated into a mesoporous graphitic sphere (MGS) support and subjected to a pore-confined growth by a subsequent high-temperature treatment, a precisely defined catalyst structure is achieved with a good H2/air performance as well as high stability towards catalyst degradation.[4]
 
 In order to correlate the impact of a precisely defined mesoporous carbon structure on the overall H2/air performance, single cell tests were performed using 5 cm2 membrane electrode assemblies (MEAs) with cathode loadings of 0.1 mgPt cmMEA
 -2 using different commercially available 20 wt.% Pt/C catalysts as well as a 28 wt.% Pt/C catalyst based on lab-scale synthesized carbon supports: i) Ketjen black (KB, TEC10E20E, TKK); ii) Vulcan (Vu, TEC10V20E, TKK); and, iii) mesoporous graphitic spheres (MGS). The latter was produced following the procedure by Knosalla et al.[5] A full MEA characterization was included to measure the electrochemically active surface area (ECSA) by CO-stripping, the H2/air performance at different operating conditions (high and low relative humidity and high pressure), the H2/O2 performance, and the O2 and H+ transport resistance in the cathode by limiting current measurements and electrochemical impedance spectroscopy (EIS), respectively. Finally, the catalyst morphology has been studied ex/situ using three/dimensional reconstruction by electron tomography and by gas adsorption measurements (argon at 87 K and water at 298 K).
 It was found, that the mesoporous carbon support significantly improves the H+ and O2 transport, resulting in an improved H2/air performance compared to both commercial catalyst materials (see. Fig. 1 MGS vs. KB or Vu). Interestingly, the MGS retains also a high ORR catalyst mass activity (imass ≈ 400 A/gPt) which is similar to the one of Pt/KB cathode catalysts (with higher internal microporous structure), leading to the good H2/air performance also at low current densities. The overall optimal performance of Pt/MGS suggests that these materials have a defined porous internal network structure which combines the beneficial effect of a facilitated O2 and H+ transport through larger mesopores while still shielding the Pt surface from ionomer contact by incorporation of Pt nanoparticles into smaller micropores.
 
 
 References:
 
 
 D. A. Cullen, K. C. Neyerlin, R. K. Ahluwalia, R. Mukundan, K. L. More, R. L. Borup, A. Z. Weber, D. J. Myers, and A. Kusoglu, Nat. Energy,
 6 (5), 462-474 (2021).
 
 
 A. Kongkanand and M. F. Mathias, J. Phys. Chem. Lett.,
 7 , 1127-1137 (2016).
 
 
 T. Lazaridis and H. A. Gasteiger, J. Electrochem. Soc.,
 168 (11), 114517 (2021).
 
 
 J. C. Meier, I. Katsounaros, C. Galeano, H. J. Bongard, A. A. Topalov, A. Kostka, A. Karschin, F. Schüth and K. J. J. Mayrhofer, Energy Environ. Sci.,
 5, 9319-9330 (2012).
 
 
 J. Knosalla, J. Mielby, D. Göhl, F.R. Wang, D. Jahlapoor, A. Hopf, K. J. J. Mayrhofer and F. Schüth, ACS. Appl. Energy Mater.,
 4, 5840-5847 (2021).
 
 
 
 
 Acknowledgement:
 
 We gratefully acknowledge funding from the German Federal Ministry for Economic Affairs and Energy (BMWi) under the funding scheme POREForm (funding number 03ET B027C).
 
 Figure 1: Measured single-cell H2/air differential flow PEMFC performance at 80°C, 95% RH, and 170 kPaabs using MEAs with Pt/C cathodes (0.1 mgPt/cm2
 MEA) based on different carbon supports: solid Vulcan carbon (Vu), porous Ketjen black (KB), or mesoporous graphitic spheres (MGS).
 
 
 
 
 
 Figure 1


Understanding the Increase in H2/Air PEM Fuel Cell Performance of Pt Based Cathode Catalysts with the Tailored Pore Structure of Mesoporous Graphitic Spheres

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Facile Solid-State Synthesis of Supported PtNi and PtCo Bimetallic Nanoparticles for the Oxygen Reduction Reaction

Stability Investigations on a Pt@HGS Catalyst as a Model Material for Fuel Cell Applications: The Role of the Local pH.

Influence of Support Material on the Structural Evolution of Copper during Electrochemical CO 2 Reduction

Insights into the Ionomer Distribution through Elemental Mapping of Model Catalysts Mixed with Nafion

Understanding the Increase in H2/Air PEM Fuel Cell Performance of Pt Based Cathode Catalysts with the Tailored Pore Structure of Mesoporous Graphitic Spheres