Acceptor Phase Research Articles

On-chip electromembrane extraction using deep eutectic solvent and red-green-blue analysis by quick-response code readable customized application on a smartphone for measuring salicylic acid in pharmaceutical and plasma samples

The current work presents an on-chip electromembrane extraction (OC-EME) method using deep eutectic solvent followed by QR code-based red-green-blue (RGB) analysis for measuring salicylic acid (SA) in plasma and pharmaceutical samples. The RGB analysis was performed based on forming the SA-Fe3+ complex in the acceptor phase giving a purple solution. The QR code readable customized app provided rapid, easy, and cost-less qualification and quantification of SA with the aid of principal component analysis (PCA). Parameters affecting OC-EME, including the supported liquid membrane (SLM), pH of the donor and acceptor phases, applied voltage, and sample flow rate, were optimized. Also, the concentration of FeCl3, as a chromogenic reagent, and its reaction time with SA were investigated to find the best concentration-dependent signal. Under the optimized conditions, a good relationship was observed between the green intensity and SA concentration within the range of 1.0–100.0 mg l−1 (R2 = 0.9946) in water and 5.0–100.0 mg l−1 (R2 = 0.9902) in plasma. Intra- and inter-day RSDs% were obtained less than 4.7% and 7.7%, respectively. Finally, the method was successfully applied for measuring SA in foot corn treatment, Aspirin medicines, and human plasma, with relative recoveries between 89.0 and 129.2%.

Drastic differences between the release kinetics of two highly related porphyrins in liposomal membranes: mTHPP and pTHPP

HypothesisThe release of hydrophobic compounds from liposomal membranes occurs by partitioning and is thus determined by the physicochemical properties (e.g. logP and water solubility) of the drug. We postulate that even minor structural differences, e.g. the position of the phenolic OH-group of the hydrophobic porphyrins mTHPP and pTHPP (meta vs. para substitution), distinctly affect their partitioning and release behavior from liposomes. ExperimentsThe release and redistribution of mTHPP and pTHPP from lecithin or POPC/POPG liposomes to different acceptor particles (DSPE-mPEG micelles and liposomes) was studied by asymmetrical flow field-flow fractionation to separate donor and acceptor particles. Reversed phase HPLC was applied to detect differences in partitioning. Molecular dynamics (MD) simulations were carried out to obtain molecular insight in the different behavior of the two compounds inside a lipid bilayer. FindingsDespite the minor differences in chemical structure, mTHPP is more hydrophobic and redistributes much slower to both acceptor phases than pTHPP. MD simulations indicate that compared to pTHPP, mTHPP makes stronger hydrogen bonds with the lipid head groups, is oriented more parallel to the lipid tails and is embedded slightly deeper in the membrane.

Solar energy-based electromembrane extraction using agarose gel for the determination of nonsteroidal anti-inflammatory drugs from biological samples: An environmentally friendly strategy

This paper presents the application of solar energy as a renewable resource in gel electromembrane extraction (G-EME). The extraction driving force (electrical field) generated from solar energy is stored through photovoltaic panels and significantly contributes to reducing the emission of greenhouse gasses. Moreover, the replacement of the polypropylene membrane and organic extracting solvents with biodegradable agarose membrane and the aqueous extracting solutions makes the presented approach compatible with the principles of green chemistry. Naproxen (NAP) and ibuprofen (IBF) were extracted from urine samples to the aqueous acceptor phase containing an anode electrode situated on the other side of the agarose gel membrane. Acceptable linearity was obtained in the concentration ranges of 6–100 and 9–100 μg. L − 1 with detection limits of 2 and 3 μg. L − 1 for NAP and IBF, respectively.

Dual‐Additive‐Driven Morphology Optimization for Solvent‐Annealing‐Free All‐Small‐Molecule Organic Solar Cells

AbstractAll‐small‐molecule organic solar cells (ASM‐OSCs), which consist of small‐molecule donors and acceptors, have recently been studied extensively to eliminate the batch‐to‐batch variation from polymer‐based donor or acceptor. On the other hand, the control of their active layer morphology is more challenging due to the similar chemical structure and miscibility of small‐molecule donor and small‐molecule accepter. Hence, this study develops a dual‐additive‐driven morphology optimization method for ASM‐OSCs based on BTR‐Cl:Y6. One solid additive – 1,4‐diiodobenzene (DIB) and one liquid additive – diiodomethane (DIM) are selected, making use of their distinct interaction mechanisms with Y6 and BTR‐Cl. It is found that DIB can form a eutectic phase with Y6, which can increase the intermolecular interactions and modulate the acceptor phase separation, while the simultaneous volatilization of DIM suppresses the over‐aggregation of BTR‐Cl during the film casting process. As a result of the synergistic morphology tuning, the optimized device delivers a power conversion efficiency (PCE) as high as 15.2%, among the highest PCE reported to date for binary ASM‐OSCs without solvent annealing treatment. This work demonstrates the potential of morphology tuning via the incorporation of dual additives into ASM‐OSCs, enabling them to achieve comparable efficiencies to those of conventional polymer/small‐molecule based OSCs.

Synthetic cathinones determination by liquid chromatography-mass spectrometry after ultrasound membrane assisted extraction

The extraction time for membrane-assisted solvent extraction (MASE) when isolating synthetic cathinones from urine has been speeded up to 30 min by using ultrasounds. Separation and determination of eleven synthetic cathinones was further performed liquid chromatography-tandem mass spectrometry (LC-MS/MS). The ultrasound assisted MASE consisted of adjusting 5.0 mL of urine at pH 11.8 and performing the extractive process with 400 μL of n-hexane as an acceptor phase inside the polypropylene membrane under ultrasonication at room temperature. Synthetic cathinones exhibiting LogP values higher than 2.0, such as 3,4-dimethyl methcathinone, methylendioxypyrovalerone, and naphyrone), were efficiently extracted and pre-concentrated. Other synthetic cathinones (LogP between 2.0 and 0.7) were found to exhibit a lower mass transfer. The method was found to be matrix dependent, and a matrix-matched calibration was required for measurements. The achieved limits of detection (LOD) were between 0.03 (flephedrone) to 0.29 (ethylone) µg L-1, with relative standard deviations (RSDs) within the 6–14% and 7–19% ranges for intraday and inter-day assays, and intraday and inter-day analytical recoveries from 84 to 115% and 85 to 118%, respectively. The developed method was finally applied to urine samples from volunteers attending a music festival.

Determination of amphetamine enantiomers in urine by conductive vial electromembrane extraction and ultra-high performance supercritical fluid chromatography tandem mass spectrometry.

Separation and quantification of amphetamine enantiomers are commonly used to distinguish between consumption of prescription amphetamine (mostly S-amphetamine) and illicit forms of the drug (racemate). In this study, electromembrane extraction with prototype conductive vials was combined with ultra-high performance supercritical fluid chromatography (UHPSFC-MS/MS) to quantify R- and S-amphetamine in urine. Amphetamine was extracted from 100 μL urine, diluted with 25 μL internal standard solution and 175 μL 130 mM formic acid, across a supported liquid membrane (SLM) consisting of 9μL of a 1:1(w/w) mixture of 2-nitrophenyloctyl ether (NPOE) and bis(2-ethylhexyl)phosphite (DEHPi) into an acceptor phase containing 300 μL 130 mM formic acid. The extraction was facilitated by the application of 30 V for 15 min. Enantiomeric separation was achieved using UHPSFC-MS/MS with a chiral stationary phase. The calibration range was 50-10,000 ng/mL for each enantiomer. The between-assay CV was ≤5%, within-assay CV ≤ 1.5%, and bias within ±2%. Recoveries were 83%-90% (CV ≤ 6%), and internal standard corrected matrix effects were 99-105 (CV ≤ 2%). The matrix effects ranged from 96% to 98% (CV ≤ 8%) when not corrected by the internal standard. The EME method was compared with a chiral routine method that employed liquid-liquid extraction (LLE) for sample preparation. Assay results were in agreement with the routine method, and the mean deviation between methods was 3%, ranging from -21% to 31%. Finally, sample preparation greenness was assessed using the AGREEprep tool, which resulted in a greenness score of 0.54 for conductive vial EME, opposed to 0.47 for semi-automated 96-well LLE.

Headspace single-drop microextraction combined with nanodrop spectrophotometry for ultra-trace detection of ethanethiol using a suspended drop of AuNPs as a plasmonic sensor

It is challenging to achieve ethanethiol extraction, enrichment in a single-drop microextraction system, and an assay with good sensitivity and selectivity for analyzing food analytes in complex matrices. In this study, we combined headspace single-drop microextraction (HS-SDME) with nanodrop array spectrophotometry applied for ultra-trace determination of ethanethiol. A suspended drop of gold nanoparticles (AuNPs) solution was utilized for sensing ethanethiol as an acceptor phase. The thiol portion of ethanethiol molecules binds to the negatively charged AuNPs. Thus, the aim of target enrichment was attained, while matrix effects interference was also minimized. The approach can be used for the direct detection of ethanethiol in food without any sample pretreatment. The obtained range of linearity was 1–1000 µM and 100–1000 nM. The detection limits were 66.62 nM, comparable with those of previously reported methods. The method successfully determined ethanethiol in food (beverage, non-alcoholic beer, and cheese).

One-Pot, Three-Phase Recycling of Metals from Li-Ion Batteries in Rotating, Concentric-Liquid Reactors.

Efficient recycling of spent lithium-ion batteries, LIBs, is essential for making their numerous applications sustainable. Hydrometallurgy-based separation methods are an indispensable part of the recycling process but remain limited by the extraction efficiency and selectivity, and typically require numerous binary liquid-liquid extraction steps in which the capacity of the extracting organic phase or partition coefficient of extracted metals become an overall bottleneck. In this paper, we describe rotating reactors in which aqueous feed, organic extractant, and aqueous acceptor phases are all present in the same, rotating vessel and can be vigorously stirred and emulsified without the coalescence of aqueous layers. In this arrangement, the extractant molecules are not equilibrated with the feed and, instead, "shuttle" between the feed/extractant and the extractant/acceptor interfaces multiple times, with each such molecule ultimately transferring ∼10 metal ions. This shuttling allows for using extractant concentrations much lower than in previous designs even for extremely concentrated feeds and, simultaneously, ensures unprecedented speed and selectivity of the one-pot processes. These experimental results are accompanied by theoretical considerations of the selectivity versus speed trends as well as discussion of parameters essential for system's upscaling. This article is protected by copyright. All rights reserved.

Isomeric acceptors incorporation enables 18.1% efficiency ternary organic solar cells with reduced trap-assisted charge recombination

The donor–acceptor miscibility is one of the most critical factors in controlling the active layer morphologies with multiple components. However, how to practically select the third component with the desired miscibility for efficient ternary organic solar cells remains unresolved. Herein, we demonstrate that the surface energy of thin films could be manipulated by altering the weight ratios of the isomeric acceptors in the blend films and, therefore, the regulation of donor–acceptor miscibility. When the acceptor weight ratio (M−Cl:O-Cl) is 1:0.3, low miscibility (χ = 5.43 × 10-2K) with PM6 is achieved, and the power conversion efficiency of organic solar cells composed of PM6:M−Cl (17.1%) is enhanced to 18.1% (PM6:M−Cl:O-Cl). The increased power conversion efficiency resulted from the surface energy-driven active layer morphology and donor–acceptor phase separations, associated with the significantly lower energetic disorder, trap density, and thus reduced free charge recombination. Our findings underline the significance of the isomeric approach to managing the blend film surface energy and, therefore, the donor–acceptor miscibility for improving the device performance, providing guidelines for the fabrication of high-performed ternary OSCs and material designs.

An improved microfluidic device to enhance the enrichment factors in liquid phase microextraction: application to the simultaneous extraction of polar and non-polar acids in biological samples

A new microfluidic device to enhance the enrichment factor in miniaturized systems is proposed. The microfluidic system was design for liquid phase microextractions, and it was applied to the simultaneous extraction of acidic compounds of a wide range of polarity (0.5 < log P < 3). The device operated under stagnant acceptor phase conditions and all the operational parameters involved were optimized. Tributyl phosphate was found to be a new highly efficient supported liquid membrane to simultaneously extract analytes of very different polarities. The optimal donor and acceptor phase were pH 2 and pH 13, respectively. The donor flow rate and the extraction time were investigated simultaneously, offering great versatility with high enrichment factors (EFs). Limits of quantitation were within 0.02 and 0.09 µg mL−1 for all compounds at 10 µL min−1 as donor flow rate and 20-min extractions, offering EFs between 11 and 18 with only 200-µL sample volume consumption. The method was successfully applied to human urine samples, observing recoveries between 47 and 90% for all compounds. This new proposed microfluidic system increases the wide range of applications, especially when the analytes are present in lower concentrations in the sample.Graphical

Green Method for the Selective Electromembrane Extraction of Parabens and Fluoroquinolones in the Presence of NSAIDs by Using Biopolymeric Chitosan Films.

A chitosan biopolymeric membrane was successfully used as a support in a green electromembrane extraction procedure for the simultaneous and selective extraction of seven parabens and three fluoroquinolones in the presence of three non-steroidal anti-inflammatory drugs. The optimal experimental conditions (10 mL donor phase and 50 μL acceptor phase, pH 10 in both phases; 80 V of applied voltage during 15 min of extraction time) were determined, providing high enrichment factors for six of the studied parabens (EF ≥ 90) and the three fluoroquinolones (EF ≥ 50). Wide linear concentration ranges (0.5-500 μg L-1), good linearity (>97%), low limits of detection (0.2-1.1 μg L-1), and good repeatability (relative standard deviation values 4-10%) were achieved. The proposed method was successfully applied for the extraction of the target analytes from different kinds of water samples (river, lake, and swimming pool). The usage of a chitosan membrane in the extraction process presents many advantages, as it is a biodegradable and versatile support, offering a good alternative to commercial plastic materials commonly used in this methodology and these procedures.

The Measurement of Hazardous Biogenic Amines in Non-Alcoholic Beers: Efficient and Applicable Miniaturized Electro-Membrane Extraction Joined to Gas Chromatography-Mass Spectrometry.

The determination of biogenic amines (BAs) as serious food contaminants and chemical indicators of unwanted microbial contamination or deficient processing conditions in non-alcoholic beers is of great interest for the beverage industries. In the present investigation, the combination of hollow fiber-electro-membrane extraction (HF-EME) and dispersive liquid-liquid microextraction (DLLME) followed by gas chromatography-mass spectrometry (GC/MS) was applied for the analysis of histamine, putrescine, tyramine, cadaverine in non-alcoholic beers. EME is fundamentally based on the electrostatic attraction, diffusion and solvability of analytes in a selected acceptor phase. This membrane-based extraction technique promoted selectivity and the enrichment factor. The DLLME process reduced the volumes of organic solvents and make the coupling of HF-EME to the CG/MS conceivable. The leading variables, which have a great effect on extraction recovery, were optimized. The relative standard deviation was achieved between 4.9 and 7.0%. The recoveries were between 94% and 98%. The limit of detection and limit of quantification were found to be 0.92-0.98 ng mL-1 and 3.03-3.23 ng mL-1, respectively. The enrichment factor was calculated in the range 36-41. The achievements revealed that putrescine and tyramine, with concentrations of 3.87 and 2.33 µg g-1, were at the highest concentration in non-alcoholic beers. This offered method with great benefits could help beverage industries to monitor the concentration of BAs in beers and control them.

A green microfluidic method for the simultaneous extraction of polar and non-polar basic compounds in biological samples

Microfluidic devices as sample treatment have showed significant advancements in recent years, becoming an important tool in pharmaceutical analysis. In this work, a green microfluidic method for the simultaneous extraction of basic polar and non-polar compounds is proposed for the first time, offering a new and more sustainable and environmentally friendly alternative. A mixture of camphor:menthol 1:1 is presented as a new green supported liquid membrane (SLM) for the simultaneous extraction of a wide log P range for basic compounds (0.4 < log P < 5): verapamil hydrochloride (VRP), tyramine (TYR), atenolol (ATN), metopropol (MTP) and nortriptyline (NRP). Different SLMs were investigated to offer new other green alternatives for polar or non-polar basic drugs. Microfluidic operational parameters were also optimized at pH 1.5, pH 11.5 and 1 µL min−1 as acceptor phase, donor phase and donor flow rate, respectively. Camphor:menthol 1:1 showed good stability and reproducibility (RSD < 5%) in human urine samples. It was found to be an attractive alternative to traditional toxic organic solvents applied in microextraction techniques. The green microfluidic method offered good recoveries between 50 and 100% for all compounds in urine sample after 7 min extraction, using only 3 µL of Ca:Me 1:1 and showing a good long-term stability system up to 6 consecutive extraction in real samples. A relative standard deviation (n = 3) was below 6 % for all compounds with and without replacing the membrane of the system.

Fabrication of a hydrophobic surface as a new supported liquid membrane for microfluidic based liquid phase microextraction device using modified boehmite nanoparticles (AlOO-NSPO)

For the first time, modified nanomaterials are introduced to the prepared polyethersulfone (PES) membrane to fabricate a hydrophobic membrane. The effectiveness of the prepared membrane in a microfluidic device based on liquid phase microextraction (LPME) was evaluated for the determination of mesalazine, an anti-inflammatory drug, in water. The PES membrane was constructed using the phase inversion method. Modified boehmite (AlOO-NSPO) nanoparticles were deposited on the surface of the PES membrane by a dip-coating method. The chemical composition and morphological study of the membrane surface and nanoparticles were characterized using field emission scanning electron microscope (FESEM), atomic force microscopy (AFM), attenuated total reflection-fourier transform infrared spectroscopy (ATR-FTIR), and static water contact angle (WCA). A significant switch from hydrophilicity to hydrophobicity was observed when the water contact angle of the membrane increased from 65.4° for PES to 97.3° for PES- (AlOO-NSPO) membrane. The performance of the new membrane and the effects of the operational parameters were evaluated in a microfluidic system based on LPME. Compared with the commercial membrane, the modified synthetic membrane with a larger pore size and porosity had a noticeable improvement under the optimum operating conditions (flow rate, 0.01 mL/min; donor phase pH, 4.5; acceptor phase pH, 12; and solvent, 1-Butanol). Furthermore, the modified membrane had an acceptable reusability, showing an extraction efficiency of 90 % after three repeated runs.

Non‐Fused Ring Acceptors Achieving over 15.6% Efficiency Organic Solar Cell by Long Exciton Diffusion Length of Alloy‐Like Phase and Vertical Phase Separation Induced by Hole Transport Layer (Adv. Energy Mater. 6/2023)

Alloy-Like Acceptors Non-fused ring electron acceptors are becoming attractive in organic solar cells due to their low cost and easy synthesis. In article number 2203402, Baomin Xu, Aung Ko Ko Kyaw, and co-workers demonstrate a ternary blend using two in-house designed non-fused ring electron acceptors and a polymer donor to form an alloy-like acceptor and vertical phase separation in the bulk-heterojunction.

An electromembrane microextraction-based green method for the determination of trace copper in natural waters.

Driven by the search for an environmentally-friendly methodology, electromembrane extraction (EME) has recently emerged as a green and versatile tool for the analysis of trace pollutants in water samples, being mainly applied to the preconcentration and determination of organic compounds. Recently, EME has also shown its applicability to the analysis of inorganic species, allowing a considerable reduction in both reagent consumption and extraction times, and without loss of efficacy, in comparison with other liquid phase microextraction techniques. In this study, an EME system for trace copper analysis in natural waters has been optimised by the modified simplex method. A chemical modifier, di-2-pyridyl ketone benzoylhydrazone (dPKBH) was synthesized and dissolved in 1-nonanol, to be used as an organic phase impregnated into the pores of a polymeric hollow fibre. With only 15 min of extraction, an enrichment factor of 77.1 ± 10.8 was obtained for a wide salinity range (0-35), allowing its application in a variety of different waters, including seawater. Optimum operating conditions were a sample pH of 6.26, an electric potential of 95 V, 0.08 M nitric acid as the acceptor phase, 4.01 mM dPKBH in 1-nonanol as the organic phase and a stirring rate of 1500 rpm. A LOD of 0.004 μg L-1 was obtained, and the system was successfully applied to the analysis of several water samples containing copper at low ppb levels (tap water and river water) or even at sub-ppb levels (seawater).

Dynamic reversed-phase liquid-liquid microextraction for the determination of Cd, Cr, Mn, and Ni in vegetable oils by energy dispersive X-ray fluorescence spectrometry

Dynamic reversed-phase liquid-liquid microextraction (RP-LLME) is proposed to prepare vegetable oil samples for posterior determination of cadmium, chromium, manganese, and nickel by energy dispersive X-ray fluorescence (EDXRF) spectrometry. The microextraction procedure was based on a dynamic system in which the sample flowed through the acceptor phase in an extraction chamber. After extraction, the rich phase was deposited on filter paper and subjected to metal determination by EDXRF. The following parameters were optimized: type and concentration of the acceptor phase, sample flow rate, and extraction time. Nitric acid 0.1 mol L−1, a sample flow rate of 10 mL min−1, and an extraction time of 15 min were employed in the recommended procedure. Under these conditions, limits of quantification of 6, 7, 8, and 11 μg kg−1 were obtained for Cd, Cr, Mn, and Ni, respectively. The preconcentration factors obtained were 100 (Cd), 65 (Cr), 82 (Mn), and 74 (Ni). The developed method was applied to determine Cd, Cr, Mn, and Ni vegetable oil samples.

Non‐Fused Ring Acceptors Achieving over 15.6% Efficiency Organic Solar Cell by Long Exciton Diffusion Length of Alloy‐Like Phase and Vertical Phase Separation Induced by Hole Transport Layer

AbstractThe construction of high‐performance organic solar cells (OSCs) based on non‐fused ring electron acceptors (NFREAs) is challenging despite their low synthesis complexity and low cost. Herein, highly efficient NFREA‐based OSCs using a ternary approach by blending two in‐house designed NFREAs called “C6C4‐4Cl” and “BTIC‐4F” with the donor PM6 are demonstrated. The two NFREAs with similar molecular skeletons tend to form an alloy‐like phase that exhibits long exciton diffusion lengths and improved crystalline properties for efficient charge transfer. The complementary absorption spectra of the ternary system and energy transfer between the two NFREAs increases the current while the high lowest unoccupied molecular orbital (LUMO) energy level of BTIC‐4F enhances the voltage of the OSCs. As a result, the ternary OSC with two NFREAs yields an impressive power conversion efficiency (PCE) of 15.62% using 2PACz as a hole transporting layer (HTL). Investigation of the buried interface reveals that 2PACz has a strong interaction with PM6 and induces vertical phase separation in the ternary blend. This work provides an effective strategy to improve the performance of NFREA‐based OSCs by increasing the exciton diffusion length in an alloy‐like acceptor phase and inducing vertical phase separation with the judicious selection of HTL.

Sensitive determination of ethosuximide in human fluids by electromembrane extraction coupled with high performance liquid chromatography ultraviolet spectroscopy

AbstractEthosuximide (ETX) is a common antiepileptic drug in the first line of absence epilepsy. In this study, for the first time, an economical and efficient electro‐membrane (EME) method for determination of ETX in a complex biological matrix using HPLC‐UV has been developed. Factors affecting conventional EME were evaluated. 1‐Octanol was immobilized in a polypropylene membrane and a voltage of 35 V was applied between two platinum electrodes for 15 min. The pH of acceptor and donor phases for ionization of ETX was adjusted to 13 and 11, respectively. Under optimal microextraction conditions, the enrichment factor was 21.02 and the linear range of ETX was 0.25 to 8.00 μg/mL with an acceptable R2 ≥ 0.9986. Inter‐day and intra‐day precision and accuracy of the suggested method were calculated with RSD &lt; 9.5% and relative error &lt;7.0%, respectively. The mean relative recovery of ETX in the human saliva and plasma samples was 81.68% and 74.47, respectively; while limit of detection and quantification concentrations were 0.08 and 0.25 μg/mL, respectively. Furthermore, to evaluate the application of the method, plasma and saliva samples of volunteers administering a single dose of ETX were analyzed successfully by EME‐HPLC‐UV method.

Nonhalogenated Solution‐Processed Donor‐Dispersed Planar Heterojunction Organic Solar Cells with Enhanced Homogeneity in Vertical Phase Separation

Realization of state‐of‐the art efficiencies in organic photovoltaics (OPV) generally relies on using toxic halogenated solution processing to arrive at the desired nanomorphology and optoelectronic responses, whereas the photovoltaic performance in nonhalogenated solution (NHS)‐based OPVs is yet nonsatisfactory, mainly related to the difficulty of morphological control. Herein, a conceptual approach of donor‐dispersed planar heterojunction (DD‐PHJ) for improving the regulation of phase morphology and photovoltaic behaviors in NHS‐processed OPVs is proposed, afforded by dispersing an ordered liquid crystal guest donor BTR‐Cl into the nonfullerene acceptor host with sequential film deposition. The combined investigation shows that the inclusion of BTR‐Cl plays a regulatory role in enhancing the crystallization, intermolecular donor/acceptor miscibility, and homogeneity in the donor–acceptor phase separation along vertical direction, which is conducive to improved charge transfer and reduced photovoltage loss. Of importance, the described DD‐PHJ approach is applicable to representative OPV material systems, leading to a champion efficiency of 18.21% in devices prepared with NHS. This work provides a promising prospect toward high‐efficiency and green solution‐processed OPV devices.