Greenificated Molecularly Imprinted Materials for Advanced Applications

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(42)

Published: June 23, 2022

Abstract Molecular imprinting technology (MIT) produces artificial binding sites with precise complementarity to substrates and thereby is capable of exquisite molecular recognition. Over five decades evolution, it predicted that the resulting host imprinted materials will overtake natural receptors for research application purposes, but in practice, this has not yet been realized due unsustainability their life cycles (i.e., precursors, creation, use, recycling, end‐of‐life). To address issue, greenificated molecularly polymers (GMIPs) are a new class plastic antibodies have approached sustainability by following one or more greenification principles, while also demonstrating far‐reaching applications compared counterparts. In review, most recent developments delicate design advanced GMIPs six fast‐growing emerging fields surveyed, namely biomedicine/therapy, catalysis, energy harvesting/storage, nanoparticle detection, gas sensing/adsorption, environmental remediation. addition, distinct features highlighted, optimal means utilize these attaining incredibly discussed. Importantly, obscure technical challenges MIT revealed, conceivable solutions offered. Lastly, several perspectives on future directions proposed.

Language: Английский

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Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4855 - 4933

Published: March 27, 2023

Heterogeneous bimetallic catalysts have broad applications in industrial processes, but achieving a fundamental understanding on the nature of active sites at atomic and molecular level is very challenging due to structural complexity catalysts. Comparing features catalytic performances different entities will favor formation unified structure-reactivity relationships heterogeneous thereby facilitate upgrading current In this review, we discuss geometric electronic structures three representative types (bimetallic binuclear sites, nanoclusters, nanoparticles) then summarize synthesis methodologies characterization techniques for entities, with emphasis recent progress made past decade. The supported nanoparticles series important reactions are discussed. Finally, future research directions catalysis based and, more generally, prospective developments both practical applications.

Language: Английский

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Chiral molecular imprinting-based SERS detection strategy for absolute enantiomeric discrimination

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Sept. 30, 2022

Abstract Chiral discrimination is critical in environmental and life sciences. However, an ideal chiral strategy has not yet been developed because of the inevitable nonspecific binding entity wrong enantiomers or insufficient intrinsic optical activities molecules. Here, we propose “inspector” recognition mechanism (IRM), which implemented on a imprinted polydopamine (PDA) layer coated surface-enhanced Raman scattering (SERS) tag layer. The IRM works based permeability change PDA after scrutiny by inspector molecule. Good enantiomer can specifically recognize fully fill cavities, whereas cannot. Then linear shape aminothiol molecule, as status introduced, only percolate through vacant nonspecifically occupied inducing SERS signal to decrease. Accordingly, chirality information exclusively stems from good specific binding, while curbed. benefits sensitivity versatility, enabling absolute wide variety molecules regardless size, functional groups, polarities, activities, scattering, number centers.

Language: Английский

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Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 13, 2023

Multimetallic alloys (MMAs) with various compositions enrich the materials library increasing diversity and have received much attention in catalysis applications. However, precisely shaping MMAs mesoporous nanostructures mapping distributions of multiple elements remain big challenge due to different reduction kinetics metal precursors complexity crystal growth. Here we design a one-pot wet-chemical approach synthesize core-shell motif PtPdRhRuCu nanospheres (PtPdRhRuCu MMNs) using diblock copolymer as soft template. The MMNs feature adjustable exposed porous structures rich highly entropic alloy sites. formation processes growth are revealed. exhibit robust electrocatalytic hydrogen evolution reaction (HER) activities low overpotentials 10, 13, 28 mV at current density 10 mA cm-2 alkaline (1.0 M KOH), acidic (0.5 H2SO4), neutral phosphate buffer solution (PBS)) electrolytes, respectively. accelerated HER derived from synergistic interactions among sites excellent mass/electron transportation characteristics.

Language: Английский

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Porous Nanoarchitectures of Nonprecious Metal Borides: From Controlled Synthesis to Heterogeneous Catalyst Applications

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(23), P. 14773 - 14793

Published: Nov. 18, 2022

Porous nonprecious metal-based nanomaterials have gained considerable attention in heterogeneous catalysis owing to their low price, high specific surface area, efficient mass/electron transfer, tunable pore structure, and unique physicochemical properties. Controlling the phase compositions of these porous materials is critical applications. transition-metal borides (TMBs), typical metal–metalloid alloys, recently received much interest because optimized electronic adjustable crystal phase, abundant active site. The controlled tuning structure TMBs, exploring relationship between performance, understanding function B are essential for developing catalysts with excellent performance; however, factors rarely been reviewed. Herein, a detailed summary synthesis methods TMBs provided by precisely defining shape, composition, size/structure. Incorporating into metals can significantly alter performance due metalloid properties B. Further, we focus on key roles related catalytic applications, including control, regulated adsorption reaction intermediates, enhanced charge transfer stability. Finally, outline shortcomings, challenges, possible development which need be further explored increase TMBs' contribution catalyst applications beyond.

Language: Английский

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A tutorial on asymmetric electrocatalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8106 - 8125

Published: Jan. 1, 2023

This tutorial review delves into the unique advantages of electrochemistry in context asymmetric catalysis, first providing a brief introduction to electrosynthesis, then exploring representative case studies with mechanistic focus.

Language: Английский

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Chiral Materials: Progress, Applications, and Prospects

Small, Journal Year: 2023, Volume and Issue: 19(38)

Published: May 22, 2023

Abstract Chirality is a universal phenomenon in molecular and biological systems, denoting an asymmetric configurational property where object cannot be superimposed onto its mirror image by any kind of translation or rotation, which ubiquitous on the scale from neutrinos to spiral galaxies. plays very important role life system. Many molecules body show chirality, such as “codebook” earth's diversity‐DNA, nucleic acid, etc. Intriguingly, living organisms hierarchically consist homochiral building blocks, for example, l ‐amino acids d ‐sugars with unknown reason. When chirality interact these chiral factors, only one conformation favors positive development life, that is, host environment can selectively conformations. The differences interactions are often manifested recognition, mutual matching, molecules, means stereoselectivity produce changes pharmacodynamics pathology. Here, latest investigations summarized including construction applications materials based natural small source, biomacromolecules sources, material synthesized design source.

Language: Английский

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New Conceptual Catalyst on Spatial High‐Entropy Alloy Heterostructures for High‐Performance Li‐O₂ Batteries

Small, Journal Year: 2023, Volume and Issue: 19(15)

Published: Jan. 8, 2023

High-entropy alloys (HEAs) are attracting increased attention as an alternative to noble metals for various catalytic reactions. However, it is of great challenge and fundamental importance develop spatial HEA heterostructures manipulate d-band center interfacial metal atoms modulate electron-distribution enhance electrocatalytic activity catalysts. Herein, efficient strategy demonstrated construct unique well-designed HEAs heterostructure electrocatalyst (HEA@Pt) bifunctional cathode accelerate oxygen reduction evolution reaction (ORR/OER) kinetics Li-O2 batteries, where uniform Pt dendrites grow on PtRuFeCoNi at a low angle boundary. Such atomically connected interfaces engender electrons from due discrepancy work functions, modulating electron distribution fast transfer, abundant active sites. Theoretical calculations reveal that redistribution manipulates atoms, allowing appropriate adsorption energy species lower ORR/OER barriers. Hence, battery based HEA@Pt delivers minimal polarization potential (0.37 V) long-term cyclability (210 cycles) under cut-off capacity 1000 mAh g-1 , surpassing most previously reported metal-based This provides significant insights electron-modulation optimization advanced electrocatalysts.

Language: Английский

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Emerging trends in chiral inorganic nanomaterials for enantioselective catalysis

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 25, 2024

Abstract Asymmetric transformations and synthesis have garnered considerable interest in recent decades due to the extensive need for chiral organic compounds biomedical, agrochemical, chemical, food industries. The field of inorganic catalysts, garnering its contributions asymmetric transformations, has witnessed remarkable advancements emerged as a highly innovative research area. Here, we review latest developments this dynamic emerging comprehensively understand advances nanocatalysts stimulate further progress catalysis.

Language: Английский

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Synthesis of Chiral Au Nanocrystals with Precise Homochiral Facets for Enantioselective Surface Chemistry

Nano Letters, Journal Year: 2022, Volume and Issue: 22(7), P. 2915 - 2922

Published: April 1, 2022

Metal surfaces with intrinsic chirality play an irreplaceable role in many significant enantioselective chemical processes such as catalysis, sensing, and separation. Nonetheless, current methods for the precise preparation of chiral suffer issues unscalable production low surface areas. Herein, we report synthesis Au nanoparticles precisely determined homochiral facets. Though a scalable wet method, {125̅8}R {85̅12}S high-Miller-index facets are obtained l- d-chiral nanocrystals, respectively. The growth process these is investigated, new nanocrystal pathway revealed. More importantly, remarkable recognition properties demonstrated enable efficient electrochemical method discrimination l-/d-tryptophan. These results provide foundation fundamental studies heterogeneous may pave way development nanocatalysts chemistry.

Language: Английский

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