ABSTRACT
Copper (Cu)-based perovskites are promising for lead-free perovskite light-emitting diodes (PeLEDs). However, it remains a significant challenge to achieve high performance devices due to the nonradiative loss caused by the disordered crystallization and lack of passivation. Crown ethers are known to form host-guest complexes by the interaction between C-O-C groups and certain cations, and 18-crown-6 (18C6) with an appropriate complementary size can interact with Cs+ and Cu+ cations. Herein, we studied the interaction between CsCu2I3 and two crowns with the same cyclic size, 18C6 and dibenzo-18-crown-6 (D18C6). Particularly, D18C6 can reduce the nonradiative recombination rate of CsCu2I3 film by passivating the defects and optimizing the film morphology effectively. The room mean square (RMS) decreased from 5.06 to 2.95 nm, and the PLQY was promoted from 4.71% to 19.9%. Besides, D18C6 can also decrease the barrier of hole injection. The PeLEDs based on D18C6-modified CsCu2I3 realized noticeable improvement with a maximum luminance and EQE of 583 cd/m2 and 0.662%, respectively.
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In organic light-emitting diode (OLED), achieving high efficiency requires effective triplet exciton confinement by carrier-transporting materials, which typically have higher triplet energy (ET) than the emitter, leading to poor stability. Here, an electron-transporting material (ETM), whose ET is 0.32 eV lower than that of the emitter is reported. In devices, it surprisingly exhibits strong confinement effect and generates excellent efficiency. Additionally, the device operational lifetime is 4.9 times longer than the device with a standard ETM, 1,3,5-tri(1-phenyl-1H-benzo[d]imidazol-2-yl) phenyl (whose ET 0.36 eV is higher than the emitter). This anomalous finding is ascribed to the exceptionally long triplet state lifetime (≈0.2 s) of the ETM. It is named as long-lifetime triplet exciton reservoir effect. The systematic analysis reveals that the long triplet lifetime of ETM can compensate the requirement for high ET with the help of endothermic energy transfer. Such combination of low ET and long lifetime provides equivalent exciton confinement effect and high molecular stability simultaneously. It offers a novel molecular design paradigm for breaking the dilemma between high efficiency and prolonged operational lifetime in OLEDs.
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To address the toxicity and stability issues of traditional lead halide perovskite solar cells (PSCs), the development of lead-free PSCs, such as Cs2AgBiBr6 solar cells, is of great significance. However, due to the low defect formation energy of Cs2AgBiBr6, a large number of vacancies, including A-site vacancies and X-site vacancies, form during the fabrication process of the Cs2AgBiBr6 film, which seriously damage the performance of the devices. The traditional phenylethylammonium (PEA) cation, mainly focusing on passivating A-site vacancies, is incapable of reducing X-site vacancies and so results in a limited performance improvement in Cs2AgBiBr6 solar cells. Herein, inspired by the capability of the Lewis base to coordinate with metal cations, a series of N-heterocyclic amines are introduced to serve as a dual-site passivator, reducing A-site and X-site vacancies at the same time. The highest power conversion efficiency of modified Cs2AgBiBr6 solar cells has been increased 36% from 1.10 to 1.50%. Further investigation reveals that the higher electron density of additives would lead to a stronger interaction with metal cations like Ag+ and Bi3+, thus reducing more X-site defects and improving carrier dynamics. Our work provides a strategy for passivating perovskite with various kinds of defects and reveals the connection between the coordination capability of additives and device performance enhancement, which could be instructive in improving the performance of lead-free PSCs.
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The emerging perovskite solar cell (PSC) technology has attracted significant attention due to its superior power conversion efficiency (PCE) among the thin-film photovoltaic technologies. However, the toxicity of lead and poor stability of lead halide materials hinder their commercialization. In this case, after a decade of effort, various categories of lead-free perovskites and perovskite-like materials have been developed, including tin halide perovskites, double perovskites, defect-structured perovskites, and rudorffites. However, the performance of the corresponding devices still falls short of expectations, especially their PCE. The limitations mainly originate from either the unstable lattice structure of these materials, which causes the distortion of their octahedra, or their low dimensionality (e.g., structural and electronic dimensionality)-correlated poor carrier transport and self-trapping effect, accelerating nonradiative recombination. Therefore, understanding the relationship between the structures and performance in these emerging candidates and leveraging these insights to design or modify new lead-free perovskites is of great significance. Herein, we review the variety of dimensionalities in different categories of lead-free perovskites and perovskite-like materials and conclude that dimensionality is an important aspect among the crucial indexes that determine the performance of lead-free PSCs. In addition, we summarize the modulation of both structural and electronic dimensionality, and the corresponding enhanced optoelectronic properties in different categories. Finally, perspectives on the future development of lead-free perovskites and perovskite-like materials for photovoltaic applications are provided. We hope that this review will provide researchers with a concise overview of these emerging materials and help them leverage dimensionality to break the bottleneck in photovoltaic applications.
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PURPOSE: The characteristics of cytokine/chemokine(CK) profiles across different courses of chronic hepatitis B virus infection and the effects of NAs antiviral therapy on cytokine profiles remain unclear. METHODS: This report provides evidence from 383 patients with chronic HBV infection. The Luminex multiple cytokine detection technology was used to detect CK profiles. The predictive power of CKs across course of disease was assessedusing univariate analyses and with receiver operating characteristic (ROC) curves. RESULTS: Compared to healthy control (HC), expression levels of interleukin 6 (IL)-6, IL-8, IL-21, matrix metalloproteinases (MMP)-2 and tumor necrosis factor receptor (TNFR)-1 showed a significant increasing trend during chronic HBV infection. IL-23 and IL-33 increased respectively in chronic hepatitis B patients (CHB). interferon (IFN)-gamma and TNF-α changed significantly only in liver cirrhosis (LC) patients. Whereas, myeloid-related markers decreased dramatically in those with hepatocellular carcinoma (HCC). The ROC result suggests that combining IL-6, IL-8, CXCL9 and CXCL13 into a nomogram has closely correlation with HCC during chronic HBV infection. In addition, nucleotide analogues (NAs) antiviral treatments are capable of recoveringnormal liver functions and significantly reducing the viral loads, however, they seem to have a limited effect in changing CKs, especially specific antiviral factors. CONCLUSION: The differential CK and virological markers may serve as potential indicators of distinct immune statuses in chronic HBV infection. They also underscore the varying efficacy and limitations of NAs antiviral therapies. This next step would to break new ground in the optimization of current anti-HBV treatment programs although this requires further research.
Subject(s)
Carcinoma, Hepatocellular , Hepatitis B, Chronic , Liver Neoplasms , Humans , Hepatitis B virus , Nucleotides , Interleukin-8 , Cytokines/metabolism , Antiviral Agents/therapeutic useABSTRACT
Inverted perovskite solar cells (PSCs) promise enhanced operating stability compared to their normal-structure counterparts1-3. To improve efficiency further, it is crucial to combine effective light management with low interfacial losses4,5. Here we develop a conformal self-assembled monolayer (SAM) as the hole-selective contact on light-managing textured substrates. Molecular dynamics simulations indicate that cluster formation during phosphonic acid adsorption leads to incomplete SAM coverage. We devise a co-adsorbent strategy that disassembles high-order clusters, thus homogenizing the distribution of phosphonic acid molecules, and thereby minimizing interfacial recombination and improving electronic structures. We report a laboratory-measured power conversion efficiency (PCE) of 25.3% and a certified quasi-steady-state PCE of 24.8% for inverted PSCs, with a photocurrent approaching 95% of the Shockley-Queisser maximum. An encapsulated device having a PCE of 24.6% at room temperature retains 95% of its peak performance when stressed at 65 °C and 50% relative humidity following more than 1,000 h of maximum power point tracking under 1 sun illumination. This represents one of the most stable PSCs subjected to accelerated ageing: achieved with a PCE surpassing 24%. The engineering of phosphonic acid adsorption on textured substrates offers a promising avenue for efficient and stable PSCs. It is also anticipated to benefit other optoelectronic devices that require light management.
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Tin-based perovskites comprise one of the preferred nontoxic alternatives to Pb-based perovskites due to their desirable optoelectronic properties. However, there remains a crucial stability problem due to the property of Sn2+ oxidation. In this study, we reported stable tin-based perovskite nanocrystals (NCs) using stannous acetate as the Sn2+ source because of its stronger Sn-O bonding. To prevent the oxidation of Sn2+, a thin layer of CsBr coverage was formed in situ; tin-based perovskite NCs, CsxSnBrx+2@CsBr (1 < x < 4), show a high photoluminescence quantum yield (PLQY) of 78.2% and high stability. The measured lifetime of PLQY decrease to half of the initial value is â¼1287 h under ambient conditions and â¼2200 h under a nitrogen atmosphere, respectively. Furthermore, the as-fabricated light-emitting diodes based on CsxSnBrx+2@CsBr NCs as the emitting layer exhibit a maximum luminescence of 16 cd/m2 and an external quantum efficiency of 0.035% with peaks at 451 and 615 nm, corresponding to the emissions of CsBr and CsxSnBrx+2, respectively. This work provided a new way to obtain stable Sn-based perovskite NCs and exhibited their potential for application in white light-emitting diodes (LEDs).
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The toxicity of lead-based halide perovskites hampers broad application in optoelectronics. The lead-free perovskite Cs2AgBiBr6 is considered a promising candidate, owing to its long carrier lifetime and outstanding stability. However, the relatively large bandgap hinders its absorption in the visible region and thus the application of its photoelectric properties in the visible and near-infrared (NIR) regions. Therefore, the expansion of absorption to the longer wavelengths, even the NIR region, makes sense for solar cells and photodetector applications. Facile elemental doping or substitution of Cs2AgBiBr6 makes it potentially desirable for applications in both visible and NIR regions. As a result, band-edge adjustment to expand the absorption onset or trace deep-energy-level doping with a new intermediate band was achieved. Here, we summarize the elemental doping results and review the potential application of Cs2AgBiBr6 from these two aspects and give constructive perspectives for further development of lead-free perovskite.
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Colloidal perovskite nanocrystals (PNCs) display bright luminescence for light-emitting diode (LED) applications; however, they require post-synthesis ligand exchange that may cause surface degradation and defect formation. In situ-formed PNCs achieve improved surface passivation using a straightforward synthetic approach, but their LED performance at the green wavelength is not yet comparable with that of colloidal PNC devices. Here, it is found that the limitations of in situ-formed PNCs stem from uncontrolled formation kinetics: conventional surface ligands confine perovskite nuclei but fail to delay crystal growth. A bifunctional carboxylic-acid-containing ammonium hydrobromide ligand that separates crystal growth from nucleation is introduced, leading to the formation of quantum-confined PNC solids exhibiting a narrow size distribution. Controlled crystallization is further coupled with defect passivation using deprotonated phosphinates, enabling improvements in photoluminescence quantum yield to near unity. Green LEDs are fabricated with a maximum current efficiency of 109 cd A-1 and an average external quantum efficiency of 22.5% across 25 devices, exceeding the performance of their colloidal PNC-based counterparts. A 45.6 h operating half-time is further documented for an unencapsulated device in N2 with an initial brightness of 100 cd m-2 .
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Background: Hepatitis B surface antigen (HBsAg) loss is considered a functional cure for chronic hepatitis B (CHB), however, several factors influence HBsAg loss. Methods: 29 CHB patients who had achieved HBsAg loss, were selected and 58 CHB patients with persistent HBsAg were matched, according to gender and age (+/- 3 years). Logistic regression and restricted cubic spline (RCS) modelling were performed. Results: Multivariate-adjusted logistic regression, based on stepwise selection, showed that baseline HBsAg levels negatively correlated with HBsAg loss (odds ratio [OR] = 0.99, 95% confidence interval [CI] = 0.98-0.99). Interferon treatment positively related with HBsAg loss (OR = 7.99, 95%CI = 1.62-44.88). After adjusting for age, HBsAg level, ALT level, HBeAg status and interferon treatment, MMP-1 (OR = 0.66, 95%CI = 0.44-0.97), CXCL9 (OR = 0.96, 95%CI = 0.93-0.99) and TNF-R1 (OR = 0.97, 95%CI = 0.94-0.99) baseline levels all negatively correlated with HBsAg loss. Our multivariate-adjusted RCS model showed that baseline CXCL10 was associated with HBsAg loss although the relationship was "U-shaped". Conclusions: Cytokines such as MMP-1, CXCL9, CXCL10 and TNF-R1 are important factors which influence HBsAg loss. It may be possible to develop a nomogram which intercalates these factors; however, further research should consider immune processes involved in HBsAg loss.
Subject(s)
Hepatitis B Surface Antigens , Hepatitis B, Chronic , Humans , Receptors, Tumor Necrosis Factor, Type I , Matrix Metalloproteinase 1 , Case-Control Studies , Hepatitis B, Chronic/drug therapy , Antiviral Agents/therapeutic use , Interferons/therapeutic use , Immunologic Factors/therapeutic use , China/epidemiologyABSTRACT
Colloidal II-VI group nanoplatelets (NPLs) possess ultranarrow emission line widths, for which they have great promise in achieving the purest display color in solution-processed light-emitting diodes (LEDs). Red NPL-LEDs have shown extremely saturated red color with high efficiency, while the green and blue ones lag far behind. Herein, we report green NPL-LEDs with the purest color in accordance with the Rec. 2020 standard and the peak external quantum efficiency (EQE) of 9.78%. By carefully controlling the aspect ratio, capping ligands, and purifications of CdSe/CdSeS core/alloyed-crown NPLs, NPL films with excellent flatness and unity photoluminescence quantum yields (PLQYs) are realized, laying a solid foundation for improving LED performance. Furthermore, via tuning the carrier injection balance, the record-high EQE for green NPL-LEDs is achieved. The electroluminescence (EL) exhibits an extremely saturated green color with the Commission Internationale de L'Eclairage (CIE) coordinates of (0.163 0.786), which demonstrates their great potential in applications of ultrahigh-definition display technology. Our findings would help to further improve the performance of all NPL-LEDs.
ABSTRACT
Colloidal semiconductor CdSe nanoplatelets (NPLs) feature ultranarrow and anisotropic emissions. However, the optical performance of blue-emitting NPLs is deteriorated by trap states, currently exhibiting tainted emissions and inferior photoluminescence quantum yields (PLQYs). Here, near trap-free blue-emitting NPLs are achieved by the controlled growth of the core/crown. Deep trap states in NPLs can be partially suppressed with the asymmetrical crown growth and are further suppressed with the growth of the small core and the alloyed symmetrical crown, yielding NPLs with pure blue emissions and near-unity PLQYs. Exciton dynamic research based on these NPLs indicates that the trap emission stems from surface traps. Besides, light-emitting diodes exhibiting ultranarrow emission centered around 461 nm with full-width-at-half-maximums down to 11 nm are fabricated using these NPLs.
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The performance degradation of perovskite solar cells (PSCs) under harsh environment (e.g., heat, moisture, light) is one of the greatest challenges for their commercialization. Herein, a conjugated sulfide 2-mercaptobenzimidazole (2MBI) is applied to significantly improve the photovoltaic properties and thermal stability of PSCs. When treated with heat, 2MBI cross-links with each other on the perovskite surface to facilitate charge transportation, suppress the escape of volatile species, and guide the rearrangement of surface perovskite grains. PSCs with 2MBI modification reach a PCE as high as 21.7% and maintain high-efficiency output during and after thermodestruction at 85 °C, while the unmodified ones suffer severe degradation. Unencapsulated devices after thermodestruction achieve over 98% of initial efficiency after 40-day storage under ambient conditions.
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All-inorganic lead-free Cs3 Cu2 I5 perovskite-derivant quantum dots (QDs) have attracted tremendous attention due to their nontoxicity and unique optoelectronic properties. However, the traditional hot-injection method requires high temperatures and multiple ligands to confine the growth of QDs. Herein, a strategy is reported to spontaneously synthesize ultrasmall Cs3 Cu2 I5 QDs within metal-organic-frameworks (MOFs) MOF-74 at room temperature (RT) with an average diameter of 4.33 nm. The obtained Cs3 Cu2 I5 QDs exhibit an evident deep-blue emission with Commission Internationale de L'Eclairage coordinates of (0.17, 0.07), owing to the strong quantum confinement effect. Due to the protection of MOF-74, the Cs3 Cu2 I5 QDs demonstrate superior stability, and the photoluminescence quantum yield retains 89% of the initial value after the storage of 1440 h under the environment with relative humidity exceeding 70%. Besides, triplet-triplet annihilation upconversion emission is observed within the composite of Cs3 Cu2 I5 @MOF-74, which brings out apparent temperature-dependent photoluminescence. This study reveals a facile method for fabricating ultrasmall lead-free perovskite-derivant QDs at RT without multiple ligands. Besides, the temperature-dependent photoluminescence of Cs3 Cu2 I5 @MOF-74 may open up a new way to develop the applications of temperature sensors or other related optoelectronic devices.
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Additive is a conventional way to enhance halide perovskite active layer performance in multiaspects. Among them, π-conjugated molecules have significantly special influence on halide perovskite due to the superior electrical conductivity, rigidity property, and good planarity of π-electrons. In particular, π-conjugated additives usually have stronger interaction with halide perovskites. Therefore, they help with higher charge mobility and longer device lifetime compared with alkyl-based molecules. In this review, the detailed effect of conjugated molecules is discussed in the following parts: defect passivation, lattice orientation guidance, crystallization assistance, energy level rearrangement, and stability improvement. Meanwhile, the roles of conjugated ligands played in low-dimensional perovskite devices are summarized. This review gives an in-depth discussion about how conjugated molecules interact with halide perovskites, which may help understand the improved performance mechanism of perovskite device with π-conjugated additives. It is expected that π-conjugated organic additives for halide perovskites can provide unprecedented opportunities for the future improvement of perovskite devices.
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The localized surface plasmon resonance (LSPR) from noble metal nanomaterials (NMs) is a promising solution to approach the theoretical efficiency for photovoltaic devices. However, the plasmon resonance of metal NMs with particular shapes and sizes can only be excited within narrow spectral ranges, which can hardly cover the broad-band solar spectrum. To address this issue, in this article, Ag NMs with irregular shapes and sizes are synthesized and embedded in the electron transport layer of perovskite solar cells. With the outstanding conductivity of Ag NMs, the series resistance and charge transfer resistance of the devices are dramatically decreased. The Ag NMs with larger size could enhance the light-trapping of the devices owing to the far-field light scattering effect. The near-field enhancement by LSPR of Ag NMs with a small size mainly contributes to the promotion of carrier transport and extraction. As a result, broad-band improvements in photovoltaic performance are achieved due to the significant enhancement of light absorption and electrical features. The highest power conversion efficiency of the perovskite solar cells increases from 19.52 to 22.42% after the incorporation of Ag NMs.
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Perovskite-based optoelectronic devices have attracted considerable attention owing to their excellent device performances and facile solution processing. However, the toxicity and intrinsic instability of lead-based perovskites have limited their commercial development. Moreover, the provision of an efficient white emission from a single perovskite layer is challenging. Here, novel electrically excited white light-emitting diodes (WLEDs) based on lead-free double perovskite Cs2 AgIn0.9 Bi0.1 Cl6 quantum dots (QDs) without any phosphor are fabricated for the first time. Density functional theory calculations are carried out to clarify the mechanism of absorption and recombination in Cs2 AgIn0.9 Bi0.1 Cl6 with Bi-doping breaking the parity-forbidden transition of the direct bandgap. Microzone optical and electronic characterizations reveal that the broadband emission of Cs2 AgIn0.9 Bi0.1 Cl6 QDs originates from self-trapped excitons, and luminescent properties are unchanged after the film deposition. The QD-WLED exhibits excellent Commission Internationale de L'Eclairage color coordinates, correlated color temperature and relatively high color rendering index of (0.32, 0.32), 6432 K, and 94.5, respectively. The maximum luminance of 158 cd m-2 is achieved by triphenylphosphine oxide passivation, and this lead-free QD-WLED exhibits a superior stability in ambient air with a long T50 ≈48.53 min. Therefore, lead-free perovskite Cs2 AgIn0.9 Bi0.1 Cl6 QDs are promising candidates for use in WLEDs in the future.
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There is growing evidence that a substantial proportion of people who complete anti-tuberculosis treatment experience significant morbidity and mortality which can negatively affect their quality of life. It is suggested that national tuberculosis programs conduct end-of-treatment assessments, but whether this is feasible is currently not known. We therefore assessed whether tuberculosis program staff could assess functional and general health status of patients at the end of treatment in five TB clinics in four provinces in China. There were 115 patients, aged 14-82 years, who completed anti-tuberculosis treatment and a post-TB assessment. There were 54 (47%) patients who continued to have symptoms, the commonest being cough, dyspnea and fatigue. Symptom continuation was significantly more common in the 22 patients with diabetes (p = 0.027) and the 12 patients previously treated for TB (p = 0.008). There were 12 (10%) current smokers, an abnormal chest X-ray was found in 106 (92%) patients and distance walked in the 6-min walking test (6MWT) ranged from 30-750 m (mean 452 ± 120); 24 (21%) patients walked less than 400 m. Time taken to perform the post-TB assessment, including the 6MWT, ranged from 8-45 min (mean 21 ± 8 min). In 98% of the completed questionnaires, health workers stated that conducting post-TB assessments was feasible and useful. This study shows that post-TB assessments can be conducted under routine programmatic conditions and that there is significant morbidity that needs to be addressed.
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BACKGROUND: We encourage Hepatitis B virus-infected mothers to breastfeed postpartum, even when continuing pregnancy category B nucleos(t)ide analogs (NAs) treatment. However, a large proportion of the Hepatitis B virus-infected mothers were noncompliant with this breastfeeding recommendation. This study aimed to investigate the factors associated with noncompliance with breastfeeding recommendation in Hepatitis B virus-infected mothers who had received NAs treatment during pregnancy. METHODS: A total of 155 mothers with chronic hepatitis B receiving NAs treatment for preventing mother-to-child transmission during the late gestation period were included and divided into exclusive breastfeeding (n = 63), mixed feeding (n = 34), and artificial feeding (n = 58) groups according to the postpartum feeding methods. Independent variables associated with feeding methods were analyzed using logistic regression analysis. RESULTS: Compared to the breastfeeding and mixed feeding groups, the artificial feeding group had significantly more multiparity, later postpartum timing of stopping NAs treatment, and a lower proportion of having knowledge of NAs medications (all P < 0.05). In addition, multivariable logistic regression analysis confirmed that multiparity, later postpartum timing of stopping NAs treatment, and lacking knowledge of medication were independent factors associated with noncompliance with breastfeeding recommendation. CONCLUSIONS: Hepatitis B virus-infected mothers who stopped NAs treatment at late postpartum period or had less knowledge of medication were more likely to be noncompliant with breastfeeding recommendation. Strengthening health education for participants taking NAs may be an important method to improve compliance with breastfeeding recommendation.
Subject(s)
Antiviral Agents/therapeutic use , Breast Feeding , Nucleosides/therapeutic use , Patient Compliance , Postpartum Period , Telbivudine/therapeutic use , Tenofovir/therapeutic use , Adult , China/epidemiology , Female , Hepatitis B, Chronic/prevention & control , Humans , Infectious Disease Transmission, Vertical/prevention & control , Pregnancy , Pregnancy Complications, Infectious/prevention & control , Retrospective Studies , Risk FactorsABSTRACT
Quasi-2D (Q-2D) perovskites are promising materials applied in light-emitting diodes (LEDs) due to their high exciton binding energy and quantum confinement effects. However, Q-2D perovskites feature a multiphase structure with abundant grain boundaries and interfaces, leading to nonradiative loss during the energy-transfer process. Here, a more efficient energy transfer in Q-2D perovskites is achieved by manipulating the crystallization kinetics of different-n phases. A series of alkali-metal bromides is utilized to manipulate the nucleation and growth of Q-2D perovskites, which is likely associated with the Coulomb interaction between alkali-metal ions and the negatively charged PbBr6 4- frames. The incorporation of K+ is found to restrict the nucleation of high-n phases and allows the subsequent growth of low-n phases, contributing to a spatially more homogeneous distribution of different-n phases and promoted energy transfer. As a result, highly efficient green Q-2D perovskites LEDs with a champion EQE of 18.15% and a maximum brightness of 25 800 cd m-2 are achieved. The findings affirm a novel method to optimize the performance of Q-2D perovskite LEDs.