Electron Acceptor Research Articles

Extracellular electron transfer genes expressed by candidate flocking bacteria in cable bacteria sediment.

Cable bacteria are ubiquitous, filamentous bacteria that couple sulfide oxidation to the reduction of oxygen at up to centimeter distances in sediment. Cable bacterial impact extends beyond sulfide oxidation via interactions with other bacteria that flock around cable bacteria and use them as electron acceptor "shortcut" to oxygen. The exact nature of this interspecies electric interaction remained unknown. With metagenomics and metatranscriptomics, we determined what extracellular electron transport processes co-occur with cable bacteria, demonstrating the identity and metabolic capabilities of these potential flockers. In sediments, microbial activities are sharply divided into anaerobic and aerobic processes, with oxygen reaching only millimeters deep. Cable bacteria extend the influence of oxygen to several centimeters, revealing a new class of anaerobic microbial metabolism with cable bacteria as electron acceptors. This fundamentally changes our understanding of sediment microbial ecology with wide-reaching consequences for sulfur, metal (in particular Fe), and carbon cycling in freshwater and marine sediments.

Hydrocarbon metabolism and petroleum seepage as ecological and evolutionary drivers for Cycloclasticus.

Aqueous-soluble hydrocarbons dissolve into the ocean's interior and structure deep-sea microbial populations influenced by natural oil seeps and spills. n-Pentane is a seawater-soluble, volatile compound abundant in petroleum products and reservoirs and will partially partition to the deep-water column following release from the seafloor. In this study, we explore the ecology and niche partitioning of two free-living Cycloclasticus strains recovered from seawater incubations with n-pentane and distinguish them as an open ocean variant and a seep-proximal variant, each with distinct capabilities for hydrocarbon catabolism. Comparative metagenomic analysis indicates the variant more frequently observed further from natural seeps encodes more general pathways for hydrocarbon consumption, including short-chain alkanes, aromatics, and long-chain alkanes, and also possesses redox versatility in the form of respiratory nitrate reduction and thiosulfate oxidation; in contrast, the seep variant specializes in short-chain alkanes and relies strictly on oxygen as the terminal electron acceptor. Both variants observed in our work were dominant ecotypes of Cycloclasticus observed during the Deepwater Horizon disaster, a conclusion supported by 16S rRNA gene analysis and read-recruitment of sequences collected from the submerged oil plume during active flow. A comparative genomic analysis of Cycloclasticus across various ecosystems suggests distinct strategies for hydrocarbon transformations among each clade. Our findings suggest Cycloclasticus is a versatile and opportunistic consumer of hydrocarbons and may have a greater role in the cycling of sulfur and nitrogen, thus contributing broad ecological impact to various ecosystems globally.

Tuning optical and electronic properties of indanthrene derivatives with electron-withdrawing groups (-Cl, -NO₂ and -C≡N) for enhanced organic solar cell performance: a DFT approach

Abstract In this study, we focused on improving the electronic and optical properties of the reference compound indanthrene (R) by introducing electron-withdrawing groups (−Cl, −C≡N, −NO₂). density functional theory and time-dependent density functional theory calculations were performed using Gaussian 16 software to study indanthrene derivatives as electron acceptor materials. The electronic and optical properties of the designed molecules (M1-M8) were investigated through frontier molecular orbital analysis, UV-visible absorption spectra, density of states, and transition density matrix analysis, utilizing GaussView 6.0 and Multiwfn 3.8 software. The designed molecules exhibit absorption across the entire visible spectrum, with maxima extending up to ~737 nm. Their electron affinity values range from 3.0 to 4.0 eV, surpassing the fullerene-based acceptor material. Among the designed molecules, M5 stands out with superior photovoltaic parameters, including a narrow optical band gap (~1.68 eV), exciton binding energy (0.25 eV), higher electron affinity (3.35 eV), an extended excited state lifetime (17.0 ns) owing to its low electron and hole reorganization energies (λe ~ 0.190 eV, and λh ~ 0.134 eV), and improved short-circuit current density of ~ 15.7 mA/cm². The photovoltaic parameters and power conversion efficiency were assessed using the Scharber and Alharbi models. The calculated device parameters, including light harvesting energy and photovoltaic characteristics (Voc, FF, Jsc, and PCE), suggest that these molecules, with electron-withdrawing groups, show great potential for use as acceptors in organic solar cells, particularly in terms of stability and power conversion efficiency. Notably, M2 and M5, with their PCE values exceeding 16%, emerge as outstanding candidates for device performance, impressively outperforming the other designed molecules.

High Color Purity Deep‐Blue Multi‐Resonance TADF Material with Narrowband Emission Toward BT.2020 Standard

AbstractDue to higher exciton energy, the deep‐blue organic light‐emitting diodes (OLEDs) are the most challenging among trichromatic emitters. In this work, three novel blue emitters with multi‐resonance (MR) effects are reported based on N,N,5,9‐tetraphenyl‐5,9‐dihydro‐5,9‐diaza‐13b‐boranaphtho[3,2,1‐de]anthracen‐7‐amine (PAB) skeleton, incorporating fluorine and methyl groups. Compound 2FPAB and MePAB exhibit ultra‐pure deep‐blue emission peaks at 436 and 448 nm respectively. The device based on MePAB achieves a maximum external quantum efficiency of 19.8% with an ultralow CIEy value of 0.046 and a full‐width‐at‐half‐maximum (FWHM) of 29 nm in the bottom emitting device. Additionally, the peripheral cladding of fluorine atoms extends the conjugation framework and slightly enhances the electron acceptance character of the boron atom at the ortho‐position. This leads to a redshift in the emission spectrum and enhanced photoluminescence quantum yield (PLQY) of up to 93% for MePABF. Furthermore, the potential application of MePAB as a deep‐blue sensitizer for MePABF is examined by fabricating a TADF‐sensitized‐TADF (TST) device. The results show a significantly reduced efficiency roll‐off and improved device performance, with a maximum external quantum efficiency (EQEmax) of 25.1% and a FWHM of 29 nm.

How the Electron-Transfer Cascade is Maintained in Chlorophyll-d Containing Photosystem I.

Photosystem I (PSI) from Acaryochloris marina utilizes chlorophyll d (Chld) with a formyl group as its primary pigment, which is more red-shifted than chlorophyll a (Chla) in PSI from Thermosynechococcus elongatus. Using the cryo-electron microscopy structure and solving the linear Poisson-Boltzmann equation, here we report the redox potential (Em) values in A. marina PSI. The Em(Chld) values at the paired chlorophyll site, [PAPB], are nearly identical to the corresponding Em(Chla) values in T. elongatus PSI, despite Chld having a 200 mV lower reduction power. The accessory chlorophyll site, A-1, in the B branch exhibits an extensive H-bond network with its ligand water molecule, contributing to Em(A-1B) being lower than Em(A-1A). The substitution of pheophytin a (Pheoa) with Chla at the electron acceptor site, A0, decreases Em(A0), resulting in an uphill electron transfer from A-1. The impact of the A-1 formyl group on Em(A0) is offset by the reorientation of the A0 ester group. It seems likely that Pheoa is necessary for A. marina PSI to maintain the overall electron-transfer cascade characteristic of PSI in its unique light environment.

Directly Fused Porphyrin-Tetracyanopentacenequinone Conjugates: Role of the Cross-Conjugated, Powerful Electron Acceptor in Promoting Highly Efficient Charge Separation.

Tetracyanopentacenequinone, a powerful electron acceptor, is fused directly to the porphyrin π-system to create a new class of donor-acceptor conjugates. Owing to the direct fusion and electron-deficient property of tetracyanopentacenequinone, strong intramolecular charge transfer both in the ground and excited states was witnessed. As a control, porphyrin fused with pentacenequinone was also investigated. Upon complete spectral and electrochemical characterization, the excited state properties were initially probed by time-dependent DFT studies, and the occurrence of electron transfer from different excited states was established. Free-energy calculations revealed higher exothermic electron transfer (> 600 mV) than the control pentacenequinone-porphyrin systems. Pump-probe studies covering broad spatial and temporal regions revealed efficient excited state charge separation. This was unlike the control pentacenequinone-porphyrin system, where slow charge separation was witnessed only in the case of the zinc derivatives but not the free-base ones. The lifetimes of the charge-separated states ranged between 30-500 ps depending on the solvent and metal ion in the porphyrin cavity. The significance of cross-conjugated tetracyanopentacenequinone fused directly to the porphyrin π system in promoting highly exothermic and efficient charge separation, irrespective of its cross conjugation, is borne out from this study.

Mechanistic Investigation of a Photoredox Cycloaddition Chain Reaction.

Photoredox catalysis is important in modern organic chemistry and the development of new synthetic methods. Mechanistic insights, particularly with photoredox chain reactions, are underdeveloped. This study combines quantum yield (QY) measurements, transient absorption spectroscopy (TAS), and electrochemical analysis to rigorously characterize the mechanism and rate constants of a ruthenium-catalyzed photoredox chain [4 + 2] cyclization between trans-anethole and isoprene. TAS and steady-state photochemical measurements (QY studies) reveal the role of oxygen in chain propagation as a secondary electron acceptor. The key kinetic competition between chain propagation and termination is identified by TAS and explored with kinetic modeling.

Fluorination Strategy for Benzimidazole Core Based Electron Acceptors Achieving over 19% Efficiency for Ternary Organic Solar Cells.

The expansion of two-dimensional conjugated systems in nonfullerene electron acceptors (NFAs) has significantly advanced the molecular design and efficiency potential of organic solar cells (OSCs). This study introduces a novel class of NFAs featuring a benzimidazole core with varying degrees of peripheral fluorination, designated as YIS-4F, YIS-6F, and YIS-8F, respectively. Through systematic modulation of fluorine content, we observed that OSCs incorporating YIS-6F achieved the highest power conversion efficiency (PCE) of 17.28%, surpassing those with YIS-4F and YIS-8F. Notably, the incorporation of YIS-6F in a ternary blend with D18/N3 yielded a remarkable PCE of 19.43%. The enhanced performance of YIS-6F-based devices is attributed to the optimized energy level alignment and optimized crystallinity, which collectively facilitate efficient exciton dissociation, accelerated charge transport, and minimized charge recombination, culminating in an exceptional fill factor and PCE. Our findings underscore the pivotal role of fluorination of NFAs at the central benzimidazole core in optimizing molecular packing, and consequently enhancing the performance of OSCs.

Nitrous oxide is the main product during nitrate reduction by a novel lithoautotrophic iron(II)-oxidizing culture from an organic-rich paddy soil.

Microbial nitrate reduction coupled to iron(II) oxidation (NRFeOx) occurs in paddy soils due to high levels of dissolved iron(II) and regular application of nitrogen fertilizer. However, to date, there is no lithoautotrophic NRFeOx isolate or enrichment culture available from this soil environment. Thus, resulting impacts on greenhouse gas emissions during nitrate reduction (i.e., nitrous oxide [N2O]) and on toxic metalloid (i.e., arsenic) mobility can hardly be investigated. We enriched a lithoautotrophic NRFeOx culture, culture HP (Huilongpu paddy, named after its origin), from a paddy soil (Huilongpu Town, China), which was dominated by Gallionella (71%). The culture reduced 0.45 to 0.63 mM nitrate and oxidized 1.76 to 2.31 mM iron(II) within 4 days leading to N2O as the main N-product (62%-88% N2O-N of total reduced NO3--N). Nitrite was present as an intermediate at a maximum of 0.16 ± 0.1 mM. Cells were associated with, but mostly not encrusted by, poorly crystalline iron(III) minerals (ferrihydrite). Culture HP performed best below an iron(II) threshold of 2.5-3.5 mM and in a pH range of 6.50-7.05. In the presence of 100 µM arsenite, only 0%-18% of iron(II) was oxidized. Due to low iron(II) oxidation, arsenite was not immobilized. However, the proportion of N2O-N of total reduced NO3--N decreased from 77% to 30%. Our results indicate that lithoautotrophic NRFeOx occurs even in organic-rich paddy soils, resulting in denitrification and subsequent N2O emissions. The obtained novel enrichment culture allows us to study the impact of lithoautotrophic NRFeOx on arsenic mobility and N2O emissions in paddy soils.IMPORTANCEPaddy soils are naturally rich in iron(II) and regularly experience nitrogen inputs due to fertilization. Nitrogen fertilization increases nitrous oxide emissions as it is an intermediate product during nitrate reduction. Microorganisms can live using nitrate and iron(II) as electron acceptor and donor, respectively, but mostly require an organic co-substrate. By contrast, microorganisms that only rely on nitrate, iron(II), and CO2 could inhabit carbon-limited ecological niches. So far, no isolate or consortium of lithoautotrophic iron(II)-oxidizing, nitrate-reducing microorganisms has been obtained from paddy soil. Here, we describe a lithoautotrophic enrichment culture, dominated by a typical iron(II)-oxidizer (Gallionella), that oxidized iron(II) and reduced nitrate to nitrous oxide, negatively impacting greenhouse gas dynamics. High arsenic concentrations were toxic to the culture but decreased the proportion of nitrous oxide of the total reduced nitrate. Our results suggest that autotrophic nitrate reduction coupled with iron(II) oxidation is a relevant, previously overlooked process in paddy soils.

Characterization and inhibition of hydrogen sulfide-producing bacteria from petroleum reservoirs subjected to alkali-surfactant-polymer flooding.

Alkali-surfactant-polymer (ASP) flooding is an emerging and promising oil recovery technique. However, the methods for preventing hydrogen sulfide-producing bacteria (SPB), chief culprits to microbial souring, in such alkali reservoirs remains unknown. Here, four alkaline-tolerant SPB exhibiting versatile sulfur metabolism were identified. Representative strains DS3, DS5, DS8, and DS23 were affiliated with Sulfurospirillum alkalitolerans, Desulfonatronovibrio hydrogenovorans, Desulfobotulus sapovorans, and Desulfovibrio alkalitolerans, respectively. Pure culture experiments showed nitrite exerted partial inhibitory effects since DS3 preferred nitrite as an electron acceptor. And nitrate inhibition was feeble, as nitrate was dissimilated to ammonium by DS3 and DS5, and DS8 preferentially utilized sulfate compared with nitrate, and DS23 ignored nitrate respiration. Glutaraldehyde effectively prevented the production of H2S in pure culture and microcosmic simulation system, demonstrating its practical application potential in alkali reservoirs. This study enhances the understanding on physiological characteristics of SPB and bridges the gap in souring management in high alkaline ASP-flooded reservoirs.

Dynamic-Cycling Zinc Sites Promote Ruthenium Oxide for Sub-Ampere Electrochemical Water Oxidation.

Although iridium-based electrocatalysts are commonly regarded as the sole stable operating acidic oxygen evolution reaction (OER) catalysts in proton-exchange membrane water electrolysis (PEMWE) devices, their exorbitant cost and scarcity severely restrict their widespread application. Herein, we introduce a promising alternative to iridium: zinc-doped ruthenium dioxide (TE-Zn/RuO2), which exhibits remarkable and enduring activity for acidic OER. In situ characterizations elucidate that the dynamic cycling of zinc dopants serves as both electron acceptors and donors, facilitating the activation of Ru sites at low overpotentials while thwarting peroxidation at high overpotentials, thus concurrently achieving heightened activity and robust stability. Additionally, the incorporation of zinc induces weakened Ru-O covalency, thereby stabling *OOH intermediates and instigating a sustained adsorbate evolution mechanism, dramatically stabilizing the RuO2 lattice. Importantly, the TE-Zn/RuO2 catalyst as an anode exhibits good stability over 300 h at a water-splitting current of 500 mA cm-2 in the PEMWE device, underscoring its considerable promise for practical applications.

Piperazine‐Functionalized Arylene Diimides as Electron Transport Layers for High‐Efficiency and Stable Organic Solar Cells

AbstractIn organic solar cells (OSCs), electron transport layer (ETL) materials are typically designed with highly polar groups to lower the work function (WF) of the cathode and ensure solvent orthogonality. However, the increased surface energy associated with these polar groups results in significant hygroscopicity and poor interfacial contact with the active layer, posing a challenge for interlayer engineering that must balance device efficiency and stability. Herein, two novel arylene diimides (PDI‐P and NDI‐P) are developed with side chains that are end‐capped with piperazine groups, as opposed to the commonly used amine groups. As ETLs, these materials not only exhibit excellent electron conductivity but also effectively lower the WF of the silver cathode. Compared to the amine‐functionalized perylene diimide (PDI‐N), the piperazine‐functionalized perylene diimide (PDI‐P) exhibits reduced surface energy and hygroscopicity, resulting in improved wettability with the active layer and decreased moisture sensitivity. These characteristics contribute to enhanced interfacial contact and device stability. The PDI‐P ETL is compatible with various high‐performance electron acceptor materials, achieving high efficiencies across a wide thickness range of ≈7 to 30 nm, with a maximum efficiency of 19.8%. These findings highlight the great potential of PDI‐P as an ETL for high‐efficiency and stable OSCs.

Co-occurrence of direct and indirect extracellular electron transfer mechanisms during electroactive respiration in a dissimilatory sulfate reducing bacterium.

Understanding the extracellular electron transfer mechanisms of electroactive bacteria could help determine their potential in microbial fuel cells (MFCs) and their microbial syntrophy with redox-active minerals in natural environments. However, the mechanisms of extracellular electron transfer to electrodes by sulfate-reducing bacteria (SRB) remain underexplored. Here, we utilized double-chamber MFCs with carbon cloth electrodes to investigate the extracellular electron transfer mechanisms of Desulfovibrio vulgaris Hildenborough (DvH), a model SRB, under varying lactate and sulfate concentrations using different DvH mutants. Our MFC setup indicated that DvH can harvest electrons from lactate at the anode and transfer them to cathode, where DvH could further utilize these electrons. Patterns in current production compared with variations of electron donor/acceptor ratios in the anode and cathode suggested that attachment of DvH to the electrode and biofilm density were critical for effective electricity generation. Electron microscopy analysis of DvH biofilms indicated DvH utilized filaments that resemble pili to attach to electrodes and facilitate extracellular electron transfer from cell to cell and to the electrode. Proteomics profiling indicated that DvH adapted to electroactive respiration by presenting more pili- and flagellar-related proteins. The mutant with a deletion of the major pilus-producing gene yielded less voltage and far less attachment to both anodic and catholic electrodes, suggesting the importance of pili in extracellular electron transfer. The mutant with a deficiency in biofilm formation, however, did not eliminate current production indicating the existence of indirect extracellular electron transfer. Untargeted metabolomics profiling showed flavin-based metabolites, potential electron shuttles.IMPORTANCEWe explored the application of Desulfovibrio vulgaris Hildenborough in microbial fuel cells (MFCs) and investigated its potential extracellular electron transfer (EET) mechanism. We also conducted untargeted proteomics and metabolomics profiling, offering insights into how DvH adapts metabolically to different electron donors and acceptors. An understanding of the EET mechanism and metabolic flexibility of DvH holds promise for future uses including bioremediation or enhancing efficacy in MFCs for wastewater treatment applications.

Redox‐Neutral Carboxylation of Benzylic Tertiary C−H Bonds with Carbon Dioxide

AbstractThe direct catalytic carboxylation of benzylic tertiary C−H bonds with CO2 for the synthesis of all‐carbon quaternary carboxylic acids represents a significant challenge. Here, we present a redox‐neutral approach to address this difficulty by leveraging the synergistic interplay between photocatalysis and cascade hydrogen abstraction cycles. Remarkably, this strategy eliminates the need for sacrificial electron donors, electron acceptors, or stoichiometric additives, offering enhanced atom economy and environmental sustainability. It is particular that the combination of α‐amino alkyl radicals with sulfur radicals generated in situ from the decomposition of DMSO was employed to realize the abstraction of benzylic tertiary C−H bonds. Our method enables the direct synthesis of a diverse array of benzylic quaternary carboxylic acids with excellent functional group tolerance as well as the derivatization of bioactive molecules and the gram‐scale synthesis of pharmaceuticals under mild reaction conditions.

Benzothiadiazole‐Fused Cyanoindone: A Superior Building Block for Designing Ultra‐Narrow Bandgap Electron Acceptor with Long‐Range Ordered Stacking

AbstractThere are great demands of developing ultra‐narrow bandgap electron acceptors for multifunctional electronic devices, particularly semi‐transparent organic photovoltaics (OPVs) for building‐integrated applications. However, current ultra‐narrow bandgap materials applied in OPVs, primarily based on electron‐rich cores, exhibit defects of high‐lying energy levels and inferior performance. We herein proposed a novel strategy by designing the benzothiazole‐fused cyanoindone (BTC) unit with ultra‐strong electron‐withdrawing ability as the terminal to synthesize the acceptor BTC‐2. The BTC unit imparts red‐shifted absorption up to 1000 nm to BTC‐2, attributed to enhanced intramolecular charge transfer and the quinoid resonance effect. Additionally, BTC‐2 features deep‐lying energy levels with the highest occupied molecular orbital level of −5.81 eV, due to the ultra‐strong electron‐withdrawing ability of BTC. Furthermore, BTC‐2 exhibits long‐range ordering in both molecular packing and macroscopic blend morphology, resulting from shoulder‐to‐shoulder packing of two BTC units, leading to an ultra‐long exciton lifetime over 1.1 ns. These superiorities facilitated a 17.17 % efficiency in the binary OPV device with an extremely high photocurrent of 30.34 mA cm−2, representing the best performance for ultra‐narrow bandgap electron acceptors, and a record light utilization efficiency of 4.88 % in binary semi‐transparent systems. Overall, BTC is a superior building block for designing ultra‐narrow bandgap electron acceptors.

Controllable Phase Separation with Star‐Shaped Y‐Type Electron Acceptors for High‐Efficiency and Stable Organic Solar Cells

Controllable Phase Separation with Star‐Shaped Y‐Type Electron Acceptors for High‐Efficiency and Stable Organic Solar Cells

Synergistically Regulating the Conjugation Length and Side Chain on Oligothiophene-Based Fully Nonfused Ring Electron Acceptors for Efficient Organic Solar Cells

Synergistically Regulating the Conjugation Length and Side Chain on Oligothiophene-Based Fully Nonfused Ring Electron Acceptors for Efficient Organic Solar Cells

The Catalytic Mechanism of a Highly Active Cobalt Chlorin Complex for Photocatalytic Water Oxidation.

Highly active catalysts for electrocatalytic and photocatalytic water oxidation are strongly demanded to realize artificial photosynthesis. A cobalt complex with a chlorin derivative ligand (CoII(Ch)) exhibited high activity for electrocatalytic water oxidation with an overpotential of 0.45 V at pH 9.0. Spectroelectrochemistry (UV-vis) unveiled the formation of two intermediates by successive one-electron oxidations. Also, the Pourbaix diagram depicted by the pH dependence of redox potentials indicated that the water oxidation proceeded after the oxidation of both the central cobalt ion and chlorin ligand with proton-coupled electron transfer (PCET). Then, the photocatalytic activity of CoII(Ch) was examined for water oxidation using [RuII(bpy)3]2+ (bpy: 2,2'-bipyridine) and S2O82- as a photosensitizer and a sacrificial electron acceptor, respectively. The turnover number, turnover frequency, and oxygen yield reached as high as 980, 5.2 s-1, and 98%, respectively, under optimized conditions. The O2-evolution rates increased in proportion to the square of the catalyst concentration in the reaction solution, suggesting that the formation of the O-O bond regarded as the rate-determining step of water oxidation proceeded by the interaction of two metal centers (I2M) mechanism in which two molecules of high-valent metal oxo or oxyl radical species react with each other.

Chemoselective Anaerobic Dehydrogenation of Alcohols By Using Visible Light and a Positively Charged Deazaflavin Catalyst Regenerated by Acetonitrile Solvent

Three series of novel deazaflavinum salts differing in their substitutions at positions 5 (R = H, phenyl or mesityl), 7 and 8 (R = OMe, Me, H or Cl) were synthesized as potential catalysts of a novel chemoselective visible light–mediated anaerobic oxidation of primary and secondary alcohols to carbonyl compounds. This mild procedure uses acetonitrile as a solvent, which acts simultaneously as a sacrificial electron acceptor (in place of the oxygen usually used in photooxidation reactions) and therefore the reaction does not need any additives. Structural and properties‐versus‐catalytic activity studies identified 5‐mesityl‐7,8‐dimethoxy‐3‐methyldeazaflavinium chloride (3a‐Cl) as the most potent catalyst. 3a‐Cl was effective in non‐deuterated acetonitrile (CH3CN), unlike its original 5‐phenyl analogue 2a‐Cl, which is efficient only in deuterated solvent (CD3CN). This difference arises because the regeneration of the 2a‐Cl catalyst is slower in CH3CN than in CD3CN. Our method using the optimized 3a‐Cl photocatalyst and CH3CN as a sacrificial oxidant and solvent in one is a useful addition to synthetic organic chemistry. Anaerobic conditions prevent side oxygenation reactions and overoxidations that usually occur in air or oxygen. This property makes this method suitable for dehydrogenations of alcohols that possess additional group(s) sensitive to oxygenation.

Suppressing Exciton-Vibration Coupling via Intramolecular Noncovalent Interactions for Low-Energy-Loss Organic Solar Cells.

Minimizing energy loss is crucial for breaking through the efficiency bottleneck of organic solar cells (OSCs). The main mechanism of energy loss can be attributed to non-radiative recombination energy loss (ΔEnr) that occurs due to exciton-vibration coupling. To tackle this challenge, tuning intramolecular noncovalent interactions is strategically utilized to tailor novel fused ring electron acceptors (FREAs). Upon comprehensive analysis of both theoretical and experimental results, this approach can effectively enhance molecular rigidity, suppress structural relaxation, reduce exciton reorganization energy, and weakens exciton-vibration coupling strength. Consequently, the binary OSC device based on Y-SeSe, which features dual strong intramolecular Se···O noncovalent interactions, achieves an outstanding power conversion efficiency (PCE) of 19.49%, accompanied by an extremely small ΔEnr of 0.184 eV, much lower than those of Y-SS and Y-SSe based devices with weaker intramolecular noncovalent interactions. These achievements not only set an efficiency record for selenium-containing OSCs, but also mark the lowest reported ΔEnr value among high-performance binary devices. Furthermore, the ternary blend device showcases a remarkable PCE of 20.51%, one of the highest PCEs for single-junction OSCs. This work demonstrates the effectiveness of intramolecular noncovalent interactions in suppressing exciton-vibration coupling, thereby achieving low-energy-loss and high-efficiency OSCs.