Technological Innovations in Photochemistry for Organic Synthesis: Flow Chemistry, High-Throughput Experimentation, Scale-up, and Photoelectrochemistry

Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(2), P. 2752 - 2906

Published: Aug. 10, 2021

Photoinduced chemical transformations have received in recent years a tremendous amount of attention, providing plethora opportunities to synthetic organic chemists. However, performing photochemical transformation can be quite challenge because various issues related the delivery photons. These challenges barred widespread adoption steps industry. past decade, several technological innovations led more reproducible, selective, and scalable photoinduced reactions. Herein, we provide comprehensive overview these exciting advances, including flow chemistry, high-throughput experimentation, reactor design scale-up, combination photo- electro-chemistry.

Language: Английский

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Sustainability Assessment of Mechanochemistry by Using the Twelve Principles of Green Chemistry

ChemSusChem, Journal Year: 2021, Volume and Issue: 14(10), P. 2145 - 2162

Published: April 9, 2021

In recent years, mechanochemistry has been growing into a widely accepted alternative for chemical synthesis. addition to their efficiency and practicality, mechanochemical reactions are also recognized sustainability. The association between Green Chemistry often originates from the solvent-free nature of most protocols, which can reduce waste production. However, satisfies more than one Principles Chemistry. this Review we will present series examples that clearly illustrate how significantly contribute fulfillment in holistic manner.

Language: Английский

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The mechanochemical synthesis of polymers

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(7), P. 2873 - 2905

Published: Jan. 1, 2022

Mechanochemistry enables solvent-free syntheses of even novel polymer structures without the need monomer solubility.

Language: Английский

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A Review on Mechanochemistry: Approaching Advanced Energy Materials with Greener Force

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(46)

Published: Jan. 11, 2022

Abstract Mechanochemistry with solvent‐free and environmentally friendly characteristics is one of the most promising alternatives to traditional liquid‐phase‐based reactions, demonstrating epoch‐making significance in realization different types chemistry. utilizes mechanical energy promote physical chemical transformations design complex molecules nanostructured materials, encourage dispersion recombination multiphase components, accelerate reaction rates efficiencies via highly reactive surfaces. In particular, mechanochemistry deserves special attention because it capable endowing materials unique properties. Herein, latest advances progress for preparation modification are reviewed. An outline basic knowledge, methods, mechanochemical strategies presented, distinguishing this review from reviews that only focus on ball‐milling. Next, followed by a detailed insightful discussion mechanochemistry‐involved conversion storage applications. The comprehensively covers aspects mechanical/optical/chemical electrical energy. Finally, next‐generation advanced proposed. This intended bring frontline guide burgeoning field interdisciplinary research developing greener force.

Language: Английский

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Ultrasound‐controlled drug release and drug activation for cancer therapy

Exploration, Journal Year: 2021, Volume and Issue: 1(3)

Published: Dec. 1, 2021

Traditional chemotherapy suffers from severe toxicity and side effects that limit its maximum application in cancer therapy. To overcome this challenge, an ideal treatment strategy would be to selectively control the release or regulate activity of drugs minimize undesirable toxicity. Recently, ultrasound (US)-responsive drug delivery systems (DDSs) have attracted significant attention due non-invasiveness, high tissue penetration depth, spatiotemporal controllability US. Moreover, US-induced mechanical force has been proven a robust method site-selectively rearrange cleave bonds mechanochemistry. This review describes US-activated DDSs fundamental basics aims present comprehensive summary current understanding US-responsive for controlled activation. First, we summarize typical mechanisms Second, main factors affecting ultrasonic responsiveness carriers are outlined. Furthermore, representative examples US-controlled activation discussed, emphasizing their novelty design principles. Finally, challenges outlook on promising therapeutic discussed.

Language: Английский

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Nanomedicine‐Enabled Sonomechanical, Sonopiezoelectric, Sonodynamic, and Sonothermal Therapy

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 22, 2023

Abstract Nanomedicine‐enabled/augmented ultrasound (US) medicine is a unique area of interdisciplinary research that focuses on designing and engineering functional nanosystems to address the challenging issues in US‐based biomedicine, overcoming shortcomings traditional microbubbles optimizing design contrast sonosensitive agents. The single‐faceted summary available US‐related therapies still significant drawback. Here, proposal comprehensive review recent advances nanomaterials advancing four biological applications disease theranostics aimed. In addition mostly explored nanomedicine‐enabled/augmented sonodynamic therapy (SDT), discussion other sono‐therapies progresses/achievements are relatively lacking, including sonomechanical (SMT), sonopiezoelectric (SPT), sonothermal (STT). concepts specific based nanomedicines initially introduced. Furthermore, representative paradigms for nanomedicine‐enabled/enhanced US elaborated according therapeutic principles diversity. This provides an updated field nanoultrasonic comprehensively discusses progress versatile ultrasonic treatments. Finally, deep facing challenges prospects expected promote emergence establishment new branch biomedicine through rational combination nanomedicine clinical biomedicine.

Language: Английский

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Ratiometric Flapping Force Probe That Works in Polymer Gels

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(6), P. 2804 - 2815

Published: Feb. 2, 2022

Polymer gels have recently attracted attention for their application in flexible devices, where mechanically robust are required. While there many strategies to produce tough by suppressing nanoscale stress concentration on specific polymer chains, it is still challenging directly verify the toughening mechanism at molecular level. To solve this problem, use of flapping force probe (FLAP) promising because can evaluate forces transmitted chain network ratiometric analysis a stress-dependent dual fluorescence. A conformational change FLAP enables real-time and reversible responses low threshold, which suitable quantifying percentage stressed chains before structural damage. However, previously reported only showed negligible response solvated environments undesirable spontaneous planarization occurs excited state, even without mechanical force. Here, we developed new that functions common organogels. Replacement anthraceneimide units wings with pyreneimide largely suppresses excited-state planarization, leading function under wet conditions. The FLAP-doped polyurethane organogel reversibly shows dual-fluorescence sub-MPa compression. Moreover, structurally modified also advantageous wide dynamic range its fluorescence solvent-free elastomers, enabling clearer imaging molecular-level during crack growth stretched film.

Language: Английский

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Polymer Mechanochromism from Force-Tuned Excited-State Intramolecular Proton Transfer

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(22), P. 9971 - 9979

Published: May 26, 2022

Real-time monitoring of strain/stress in polymers is a big challenge to date. Herein, we for the first time report an ESIPT (excited-state intramolecular proton transfer)-based mechanochromic mechanophore (MM). The synthesis target MM PhMz-4OH [(2-hydroxyphenyl)benzimidazole with four aliphatic hydroxyls] quite facile. possesses characteristic dual emissions, and its activity greatly affected by steric hindrance. Then, was covalently linked into polyurethane chains (PhMz-4OH@PU). Upon stretching, PhMz-4OH@PU films showed fluorescence color change spectral variation increase enol emission blueshift keto due force-induced torsion dihedral angle between donor acceptor. high concentrations (>0.36 mol %) might undergo two-stage force-responsive process, including via disaggregation direct chain-transduced angle. intensity ratio (IE/IK) shows quantitative correlation elongation, real-time strain sensing achieved. successful type II (without covalent bond scission) displays sensitivity excellent reversibility stress. Two control structures PhMz-NH2 PhMz-2OH were also embedded PU but no or changes detected, further confirming that mechanochromism arises from force. Density function theory (DFT) calculation performed study force-tuned process theoretically rationalize experimental results. This lay foundation stress/strain practical applications.

Language: Английский

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Covalent Mechanochemistry and Contemporary Polymer Network Chemistry: A Marriage in the Making

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(2), P. 751 - 768

Published: Jan. 4, 2023

Over the past 20 years, field of polymer mechanochemistry has amassed a toolbox mechanophores that translate mechanical energy into variety functional responses ranging from color change to small-molecule release. These productive chemical changes typically occur at length scale few covalent bonds (Å) but require large inputs and strains on micro-to-macro in order achieve even low levels mechanophore activation. The minimal activation hinders translation available materials device applications. challenge inspires core questions yet another control, namely: What are molecular-scale features polymeric material determine extent activation? Further, how do we marry advances chemistry networks with create stress-responsive well suited for an intended application? In this Perspective, speculate as potential match between recent network chemistry, specifically, topologically controlled hierarchical enabled by multi-network architectures mechanically interlocked polymers. Both fundamental applied opportunities unique union these two fields discussed.

Language: Английский

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Outstanding Advantages, Current Drawbacks, and Significant Recent Developments in Mechanochemistry: A Perspective View

Crystals, Journal Year: 2023, Volume and Issue: 13(1), P. 124 - 124

Published: Jan. 10, 2023

Although known since antiquity, mechanochemistry has remained dormant for centuries. Nowadays, is a flourishing research field at the simultaneous stages of gathering data and (often astonishing) observations, scientific argumentation toward their analysis, which combination interdisciplinary expertise necessary. Mechanochemistry’s implementation as synthetic method constantly increasing, although it remains far from being fully exploited, or understood on basis fundamental principles. This review starts by describing many remarkable advantages mechanochemical reactions, simplifying “greening” chemistry in solutions. description followed an overview current main weaknesses to be addressed near future systematic study its energetics chemical mechanisms. finishes recent breakthrough experimental advances, such situ kinetics monitoring using synchrotron X-ray powder diffraction Raman spectroscopy, plus equally significant computational approaches, quantum mechanochemistry, used understanding covalent hydrogen bond ruptures biomolecules mechanophores polymers single-molecule level. Combined with new technologies control temperature pressure ball mills, these appealing methods are promising tools establishing knowledge necessary reactivity

Language: Английский

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