Abstract:Emerging charge-functional electronic and electrochemical materials exhibit increasingly complex structure. Critical fundamental processes (e.g., charge transport, electrocatalysis) must work cooperatively across multiple time-and length scales to realize desired properties. Performance optimization in these materials demands an ultimate multifaceted, multiscale understanding of structure versus charge-function relationships, in order to address longstanding challenges associated with, for example, climate cha… Show more
“…17 In these materials, many charge-functional processes, such as electron conduction, ionic adsorption, and surface redox reactions, occur simultaneously and interact strongly with one another, dictating the overall water treatment performances, including ion selectivity, cycle stability, removal capacity and rate. 18,19 Rationally designed charge-functional materials with high water treatment performance display increasingly complex structure and functionality, demanding multifaceted characterizations of critical processes (e.g., charge transport and surface catalysis) across multiple length and time scales. 17 While conventional techniques such as electron microscopy and X-ray photoelectron spectroscopy can offer important information such as materials morphology and chemical compositions, such multiscale understanding of highly complex systems demands the development of in situ, operando characterization tools with high spatiotemporal resolutions that can, for example, capture kinetic phenomena during electrochemical operations 20,21 and quantify local functional parameters (e.g., charge carrier mobility and electrocatalytic activity).…”
Section: List Of Symbolsmentioning
confidence: 99%
“…Imaging charge transport.-Electronic and ionic transport in charge-functional materials significantly affect the redox reactions at the electrode/electrolyte interface, governing the key performance metrics for electrochemical mediated water remediation such as selectivity, capacity and rate. 18 For instance, the mobility or diffusion length of photogenerated charge carriers in semiconductors affects electron-hole separation, which in turn controls the surface hole/electron activities toward photoelectrochemical oxidative pollutant decomposition. 37 The forms (e.g., hydrated ions) and valences (e.g., monovalent, divalent and trivalent) of intercalated ions have a critical impact on the ion removal capacity and rate capability in water deionization processes.…”
Section: In Situ Operando Imaging For Understanding Electrochemical W...mentioning
confidence: 99%
“…High spatiotemporal resolution imaging in realistic liquid environments (i.e., multiple species of varying concentrations) can be powerful tools to probe the critical underlying dynamic processes ( i.e., surface restructuring, interface instability, time-dependent molecular binding). Particularly, functional imaging techniques 18,22,98,105,122 can quantitatively probe local charge function such as pollutant adsorption strength and carrier mobility, and thus should be leveraged to build local structure-activity relationship in emerging water treatment electrodes of highly complex, heterogeneous structures and morphologies, providing insights complementary to those from structural imaging to yield a holistic picture of fundamental processes and mechanisms that govern water treatment efficiency. For instance, the complex water matrix will lead to ion co-insertion and surface passivation of electrode materials, detrimental to electrode cycle stability and target ions selectivity.…”
Section: In Situ Operando Imaging For Understanding Electrochemical W...mentioning
Water management by electrochemical means has attracted increasing attention due to the high energetic efficiency and significantly improved water treatment efficacy of related emerging technologies. Charge functions in electronic and electrochemical materials dictate the overall water treatment performance such as selectivity, operation stability, removal capacity, and rate. Here, we elucidate the design principles of charge-functional materials for electrochemically mediated water treatment by considering fundamental performance-governing processes, including charge transport, surface adsorption, bulk ion insertion, and (photo)electrocatalysis. Furthermore, we highlight the recent development of in situ operando imaging tools for probing these critical processes that occur during water treatment, with a particular focus on functional imaging techniques capable of probing local charge-functional parameters (e.g., charge carrier diffusivity, pollutant adsorption affinity, and redox reaction rate) to establish local structure-function relationships. We conclude this review by pointing out the opportunities and challenges that warrant future research in order to further improve the performance and scale-up ability of electrochemical water treatment technologies in the broader context of the energy-environment nexus toward a sustainable zero-carbon future.
“…17 In these materials, many charge-functional processes, such as electron conduction, ionic adsorption, and surface redox reactions, occur simultaneously and interact strongly with one another, dictating the overall water treatment performances, including ion selectivity, cycle stability, removal capacity and rate. 18,19 Rationally designed charge-functional materials with high water treatment performance display increasingly complex structure and functionality, demanding multifaceted characterizations of critical processes (e.g., charge transport and surface catalysis) across multiple length and time scales. 17 While conventional techniques such as electron microscopy and X-ray photoelectron spectroscopy can offer important information such as materials morphology and chemical compositions, such multiscale understanding of highly complex systems demands the development of in situ, operando characterization tools with high spatiotemporal resolutions that can, for example, capture kinetic phenomena during electrochemical operations 20,21 and quantify local functional parameters (e.g., charge carrier mobility and electrocatalytic activity).…”
Section: List Of Symbolsmentioning
confidence: 99%
“…Imaging charge transport.-Electronic and ionic transport in charge-functional materials significantly affect the redox reactions at the electrode/electrolyte interface, governing the key performance metrics for electrochemical mediated water remediation such as selectivity, capacity and rate. 18 For instance, the mobility or diffusion length of photogenerated charge carriers in semiconductors affects electron-hole separation, which in turn controls the surface hole/electron activities toward photoelectrochemical oxidative pollutant decomposition. 37 The forms (e.g., hydrated ions) and valences (e.g., monovalent, divalent and trivalent) of intercalated ions have a critical impact on the ion removal capacity and rate capability in water deionization processes.…”
Section: In Situ Operando Imaging For Understanding Electrochemical W...mentioning
confidence: 99%
“…High spatiotemporal resolution imaging in realistic liquid environments (i.e., multiple species of varying concentrations) can be powerful tools to probe the critical underlying dynamic processes ( i.e., surface restructuring, interface instability, time-dependent molecular binding). Particularly, functional imaging techniques 18,22,98,105,122 can quantitatively probe local charge function such as pollutant adsorption strength and carrier mobility, and thus should be leveraged to build local structure-activity relationship in emerging water treatment electrodes of highly complex, heterogeneous structures and morphologies, providing insights complementary to those from structural imaging to yield a holistic picture of fundamental processes and mechanisms that govern water treatment efficiency. For instance, the complex water matrix will lead to ion co-insertion and surface passivation of electrode materials, detrimental to electrode cycle stability and target ions selectivity.…”
Section: In Situ Operando Imaging For Understanding Electrochemical W...mentioning
Water management by electrochemical means has attracted increasing attention due to the high energetic efficiency and significantly improved water treatment efficacy of related emerging technologies. Charge functions in electronic and electrochemical materials dictate the overall water treatment performance such as selectivity, operation stability, removal capacity, and rate. Here, we elucidate the design principles of charge-functional materials for electrochemically mediated water treatment by considering fundamental performance-governing processes, including charge transport, surface adsorption, bulk ion insertion, and (photo)electrocatalysis. Furthermore, we highlight the recent development of in situ operando imaging tools for probing these critical processes that occur during water treatment, with a particular focus on functional imaging techniques capable of probing local charge-functional parameters (e.g., charge carrier diffusivity, pollutant adsorption affinity, and redox reaction rate) to establish local structure-function relationships. We conclude this review by pointing out the opportunities and challenges that warrant future research in order to further improve the performance and scale-up ability of electrochemical water treatment technologies in the broader context of the energy-environment nexus toward a sustainable zero-carbon future.
“…[1][2][3] In chemical laboratories, exploring and optimizing chemical compounds are commonly performed for functionalizing and novelizing them by experts with professional knowledge. [4][5][6][7][8][9][10][11][12][13][14][15] A vast amount of knowledge has been accumulated to facilitate the exploration and optimization processes in the long history of chemistry. 1 Meanwhile, the vast amount of knowledge complicates and perplexes these processes, which causes numerous trial-and-error routines even for the experts.…”
Section: Introductionmentioning
confidence: 99%
“…Controlling phenomena and properties of molecules at the atomic level is a challenging task 1–3 . In chemical laboratories, exploring and optimizing chemical compounds are commonly performed for functionalizing and novelizing them by experts with professional knowledge 4–15 . A vast amount of knowledge has been accumulated to facilitate the exploration and optimization processes in the long history of chemistry 1 .…”
Designing functional molecules is the prerogative of experts who have advanced knowledge and experience in their fields. To democratize automatic molecular design for both experts and nonexperts, we introduce a generic open‐sourced framework, ChemTSv2, to design molecules based on a de novo molecule generator equipped with an easy‐to‐use interface. Besides, ChemTSv2 can easily be integrated with various simulation packages, such as Gaussian 16 package, and supports a massively parallel exploration that accelerates molecular designs. We exhibit the potential of molecular design with ChemTSv2, including previous work, such as chromophores, fluorophores, drugs, and so forth. ChemTSv2 contributes to democratizing inverse molecule design in various disciplines relevant to chemistry.This article is categorized under:
Data Science > Databases and Expert Systems
Data Science > Artificial Intelligence/Machine Learning
Data Science > Computer Algorithms and Programming
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