ACS Applied Energy Materials最新文献

{"title":"Enhanced Electrochemical Nitrogen Reduction via the Transport of Superacidic Microdroplets","authors":"Amir H. Aslambakhsh, Yuecheng Zhang, Sandra E. Kentish, Colin A. Scholes","doi":"10.1021/acsaem.4c01575","DOIUrl":"https://doi.org/10.1021/acsaem.4c01575","url":null,"abstract":"Electrocatalysts with a small overpotential hold a clear advantage in energy conversion efficiency. However, in electrochemical nitrogen reduction reactions (eNRRs), the primary challenge remains the issue of low selectivity. This study presents a gas-through cell assembly for eNRR to advance sustainable ammonia synthesis. The assembly introduces superacidic microdroplets via nitrogen gas, enhancing nitrogen concentration on the catalyst surface and amplifying nitrogen electrofixation rates. Catalyst deposition on a gas diffusion layer surface with a hydrophobic polymer binder enables microdroplet delivery to the working electrode surface through an ultrasonic nebulizer. Investigating parameters such as flow rate, water microdroplet content, temperature, pH, and applied potential provides valuable insights into eNRR performance. Unlike conventional H-cell setups, the proton concentration of the nebulizer flow emerges as the primary limiting factor in the gas-through cell assembly, impacting ammonia yield rate and Faradaic efficiency. Superacidic droplets enhance ammonia production, but further reducing pH increases hydrogen generation, lowering Faradaic efficiency toward ammonia. Higher temperatures accelerate ammonia production but reduce the Faradaic efficiency due to increased competition from the hydrogen evolution reaction, while elevated potentials initially boost eNRR but drop selectivity due to competing reactions. An optimum ammonia yield rate and Faradaic efficiency of 24.2 ± 2.4 <i></i><span style=\"color: inherit;\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\"><mi>μ</mi><msub><mi mathvariant=\"normal\">g</mi><mrow><msub><mi>NH</mi><mn>3</mn></msub></mrow></msub><msup><msub><mi>mg</mi><mrow><mi>cata.</mi></mrow></msub><mrow><mo>−</mo><mn>1</mn></mrow></msup><msup><mi mathvariant=\"normal\">h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math>' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span style=\"width: 8.185em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 7.446em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.31em, 1007.45em, 2.787em, -999.997em); top: -2.327em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝜇</span><span><span style=\"display: inline-block; position: relative; width: 1.878em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.355em, 1000.46em, 4.378em, -999.997em); top: -3.974em; left: 0em;\"><span style=\"font-family: STIXMathJax_Main;\">g</span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absol","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142188132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Facile Design and Synthesis of Co-Free Layered P2-Na2/3Fe1/2Mn1/2O2 as Advanced Cathode Material for Sodium-Ion Batteries","authors":"Lixiong Qian,&nbsp;Rui Huang,&nbsp;Haoran Zhang,&nbsp;Shengxue Yan and Shaohua Luo*,&nbsp;","doi":"10.1021/acsaem.4c0191510.1021/acsaem.4c01915","DOIUrl":"https://doi.org/10.1021/acsaem.4c01915https://doi.org/10.1021/acsaem.4c01915","url":null,"abstract":"<p >Co-free Fe/Mn-based cathodes have become a popular choice for sodium-ion batteries (SIBs) due to their affordability and impressive theoretical capacity. Nevertheless, the issue of their terrible battery life and rate capability continues to be their hindrances. A set of three-factor, three-level orthogonal experiments was adopted, including the calcination temperature, calcination time, and heating rate. And two single-factor experiments were carried out to further optimize the preparation conditions. Finally, the optimal conditions were obtained as follows: the calcination temperature was 900 °C, the calcination time was 12 h, and the heating rate was 5 °C min^–1. The layered oxide cathode material Co-free P2-Na_2/3Fe_1/2Mn_1/2O₂ was synthesized by the solid phase method. Under the control of the optimal conditions, the P2-Na_2/3Fe_1/2Mn_1/2O₂ cathode could yield a remarkable initial discharge specific capacity (179.3 mAh g^–1, 0.1 C) and cycle stability (54.6% over 50 cycles). These findings further declared that it was feasible to design Co-free Fe/Mn-based cathode materials with superior performance, which might offer guidance for popularizing cost-effective Fe/Mn-based cathode materials in the future.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276318","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Electrochemical Nitrogen Reduction via the Transport of Superacidic Microdroplets","authors":"Amir H. Aslambakhsh,&nbsp;Yuecheng Zhang,&nbsp;Sandra E. Kentish and Colin A. Scholes*,&nbsp;","doi":"10.1021/acsaem.4c0157510.1021/acsaem.4c01575","DOIUrl":"https://doi.org/10.1021/acsaem.4c01575https://doi.org/10.1021/acsaem.4c01575","url":null,"abstract":"<p >Electrocatalysts with a small overpotential hold a clear advantage in energy conversion efficiency. However, in electrochemical nitrogen reduction reactions (eNRRs), the primary challenge remains the issue of low selectivity. This study presents a gas-through cell assembly for eNRR to advance sustainable ammonia synthesis. The assembly introduces superacidic microdroplets via nitrogen gas, enhancing nitrogen concentration on the catalyst surface and amplifying nitrogen electrofixation rates. Catalyst deposition on a gas diffusion layer surface with a hydrophobic polymer binder enables microdroplet delivery to the working electrode surface through an ultrasonic nebulizer. Investigating parameters such as flow rate, water microdroplet content, temperature, pH, and applied potential provides valuable insights into eNRR performance. Unlike conventional H-cell setups, the proton concentration of the nebulizer flow emerges as the primary limiting factor in the gas-through cell assembly, impacting ammonia yield rate and Faradaic efficiency. Superacidic droplets enhance ammonia production, but further reducing pH increases hydrogen generation, lowering Faradaic efficiency toward ammonia. Higher temperatures accelerate ammonia production but reduce the Faradaic efficiency due to increased competition from the hydrogen evolution reaction, while elevated potentials initially boost eNRR but drop selectivity due to competing reactions. An optimum ammonia yield rate and Faradaic efficiency of 24.2 ± 2.4 <i></i><math><mi>μ</mi><msub><mi>g</mi><mrow><msub><mi>NH</mi><mn>3</mn></msub></mrow></msub><msup><msub><mi>mg</mi><mrow><mi>cata.</mi></mrow></msub><mrow><mo>−</mo><mn>1</mn></mrow></msup><msup><mi>h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math> and 27 ± 4.4% were achieved, with 50 mL/min total flow rate and 50% volume microdroplet content, respectively; the ammonia synthesis rate reached as high as 37.6 ± 4 <i></i><math><mi>μ</mi><msub><mi>g</mi><mrow><msub><mi>NH</mi><mn>3</mn></msub></mrow></msub><msup><msub><mi>mg</mi><mrow><mi>cata.</mi></mrow></msub><mrow><mo>−</mo><mn>1</mn></mrow></msup><msup><mi>h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math> at 85 °C, while the best Faradaic efficiency of 58.2 ± 9.3% was observed at pH = 2.8 ± 0.1 under −2 V applied potential and ambient pressure. This study enhances our understanding of gas-through electrochemical nitrogen fixation, providing invaluable insights for the development of efficient and sustainable ammonia synthesis strategies.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High Selectivity in CO2 Reduction to CO Using Metal-Decorated C3N4 Nanotubes","authors":"Chi-You Liu, Elise Yu-Tzu Li","doi":"10.1021/acsaem.4c01922","DOIUrl":"https://doi.org/10.1021/acsaem.4c01922","url":null,"abstract":"An important aspect of the CO₂ reduction reaction (CO2RR) is to inhibit the H₂ evolution reaction (HER) at the electrodes and to increase the formation of other valuable carbon products. In principle, a higher CO product selectivity allows for a higher amount of C₂₊ products in the CO2RR. Here, we report a material, the metal-decorated C₃N₄ nanotubes (M_<i>n</i>/CNNTs, <i>n</i> = 1 and 4), which exhibits high CO selectivity and low HER probabilities. Our DFT calculations indicate that this catalyst system strongly activates the CO₂ molecule through a unique adsorption site on the surface, which then undergoes the COOH intermediate transformation to CO. The results show that the single Fe or Cu atom combined with the armchair-type CNNTs shows the best CO selectivity with low CO2RR overpotentials (&lt;0.4 V), signifying an opportunity for efficient and economical CO₂ conversion for future applications.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142188124","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Study of Lithium Transport in NMC Layered Oxide Cathode Material Using Multiscale Computational Approach","authors":"Ali Jaberi*,&nbsp;Michel L. Trudeau,&nbsp;Jun Song and Raynald Gauvin*,&nbsp;","doi":"10.1021/acsaem.4c0111310.1021/acsaem.4c01113","DOIUrl":"https://doi.org/10.1021/acsaem.4c01113https://doi.org/10.1021/acsaem.4c01113","url":null,"abstract":"<p >Enhancing the rate capability of lithium-ion batteries (LIBs), as a promising energy storage device, requires a comprehensive understanding of lithium (Li) transport in their constituent parts. In this study, Li transport in the LiNi_0.333Mn_0.333Co_0.333O₂ (NMC111) cathode active material was examined by a multiscale computational approach ranging from density functional theory (DFT) to Monte Carlo (MC) simulations. The approach was first applied to lithium cobalt oxide (LCO) to compare our model with an existing available one for barrier energies in layered structures. Two barrier energy models, named the interpolated barrier model and the local cluster expansion, together with the periodic cluster expansion, were integrated into the KMC algorithm. Results of KMC simulations in LCO were similar using both barrier models. Thus, the approach was then applied to NMC111 by using only the much simpler interpolated barrier model. Our MC simulations showed a perfect honeycomb-like ordering of Li ions in the Li layer of NMC111 at a Li concentration of 0.8. This perfect ordering of Li ions caused a significant decrease in the thermodynamic factor, which consequently resulted in a minimum in the chemical diffusion coefficient at this concentration, confirming previous studies. The perfect correlation between our simulations and the experimental measurements of other studies reflects the precision of our formalism in studying the transport behavior of Li in the NMC111 crystal.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276313","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthetically Enforced Cation Migration in Sillén–Aurivillius Hybrid Perovskites Boosts Photocatalytic Hydrogen Evolution","authors":"Shubham Kumar,&nbsp;Jaideep Malik,&nbsp;Anil Kumar,&nbsp;Parul Yadav and Tapas Kumar Mandal*,&nbsp;","doi":"10.1021/acsaem.4c0166910.1021/acsaem.4c01669","DOIUrl":"https://doi.org/10.1021/acsaem.4c01669https://doi.org/10.1021/acsaem.4c01669","url":null,"abstract":"<p >Sillén–Aurivillius (S–A) hybrid layered perovskites constitute an important class of intergrowth compounds that have been recently demonstrated as high-performing semiconductor photocatalysts. The present study reports the synthesis of a series of three-layer S–A perovskites (A3X1 hybrids), Bi₄AA′Ti₂NbO₁₄Cl (A, A′ = Sr and Ba), by an innovative approach involving interchange of Sr and Ba between the starting Sillén and Aurivillius blocks to examine the cation redistribution in the resulting intergrowth phases. Rietveld structure refinements reveal the preferred occupation of Sr in the perovskite block, while the larger Ba is grounded in the Sillén block. Due to cation migration between the fluorite-like [Bi₂O₂] layer and the perovskite block during intergrowth formation, the projected composition Bi₄Ba_[P]Sr_[S]Ti₂NbO₁₄Cl (where [P] indicates the perovskite block, while [S] indicates the fluorite block) evolves into the phase with a mixed cation distribution, Bi₄Ba_0.1[P]Sr_0.9[P]Ba_0.9[S]Sr_0.1[S]Ti₂NbO₁₄Cl. The cation migration appears to improve the packing by simultaneously reducing the height of the perovskite block and decreasing the divergence in the Bi–O bond lengths of the fluorite block simultaneously. This leads to greater mixing of Ti-3d, Nb-4d, and Bi6p states contributing near the conduction band minima. The cation-migrated S–A hybrid shows enhanced photocatalytic hydrogen evolution (PHE) as compared to the hybrid perovskites with nonmigrated or unmixed cation distribution. The present investigation discusses the innovative synthesis, cation migration, site disorder, and first-principles electronic structure calculations to unveil their role in enhanced PHE.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Direct Ion-Exchange Method for Preparing a Solution Allowing Spontaneous Perovskite Passivation via Hole Transport Material Deposition","authors":"Naoyuki Nishimura, Hiroyuki Kanda, Takurou N. Murakami","doi":"10.1021/acsaem.4c01314","DOIUrl":"https://doi.org/10.1021/acsaem.4c01314","url":null,"abstract":"We propose a direct ion-exchange (DI) method for preparing a hole transport material (HTM) solution undergoing spontaneous perovskite passivation via HTM deposition and verify its applicability for the photovoltaic performance enhancement of perovskite solar cells (PSCs). The simple synthesis of a Spiro-OMeTAD HTM solution based on ion exchange via dissolving and mixing multiple solid materials in a chlorobenzene solution produces an HTM solution similar to that obtained with an <i>n</i>-octylammonium bis(trifluoromethanesulfonyl)imide ionic liquid functioning as a spontaneous perovskite passivator. Using the resulting HTM solution, the power conversion efficiency of PSCs was enhanced up to 23.0% without conventional postpassivation processes.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142188121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Porous Hollow Carbon Alkali-Activated Nanoonions As a Conductive Additive for High-Rate Lithium Primary Batteries","authors":"Guilu Qin, Yifan Liu, JiaCheng He, Nengkun Wang, Junwei Wang, Xian Jian","doi":"10.1021/acsaem.4c01531","DOIUrl":"https://doi.org/10.1021/acsaem.4c01531","url":null,"abstract":"The high content of the covalent C–F bond of CF_<i>x</i> materials makes the conductivity of the materials worse and the battery polarization serious, which greatly reduces power density and leads to heat generation. Therefore, adding a conductive agent is particularly important, as it improves the electron migration speed in the electrode, suppresses the polarization phenomenon, and promotes the effective use of active substances. In this paper, a carbon nanoonion (CNO) with a hollow porous structure is prepared by a room-temperature alkaline activation method as a conductive agent for the Li/CF_<i>x</i> battery. The porous structures reduce the diffusion resistance of lithium ions, which is beneficial for Li/CF_<i>x</i> batteries to achieve a better rate performance. The electrochemical results show that alkali-activated CNO as a part of the cathode material effectively improves the rate performance of the Li/CF_<i>x</i> batteries. At the 2 C discharge rate, the specific capacity and energy density of CNO-NaOH-5M increased by 83.59% and 144.63%, respectively, compared with the commercial conductive additive SP. The power density and energy density of CNO-NaOH-3M samples at 8 C are 6907.36 and 863.42 Wh/kg, respectively, which was significantly better than the original CNO and SP. As a conductive agent, the increase of the oxygen-containing functional group of alkali-activated CNO improves the infiltrability of the cathode to the electrolyte, and the increase of pore-hollow structure improves the interface contact area, which is conducive to the transmission speed of electrons and lithium ions during discharge so that the Li/CF_<i>x</i> battery has high rate performance.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142224617","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Valence State Regulated Nickel Iron Layered Double Hydroxides by Amine Intercalation as Efficient Electrocatalysts for Seawater Oxidation","authors":"Sakila Khatun, Poulomi Roy","doi":"10.1021/acsaem.4c00979","DOIUrl":"https://doi.org/10.1021/acsaem.4c00979","url":null,"abstract":"The manipulation of the valence state along with electronic spin configurations of metal sites in NiFe layered double hydroxides has been recognized as a feasible strategy to boost intrinsic electrocatalytic oxygen evolution reaction activity. In this study, high-valence Ni³⁺ with a low-spin configuration has been introduced in NiFe layered double hydroxide nanosheets by facile amine intercalation in the interlayers. The influence of such valence state regulations with a favorable electronic low-spin configuration of Ni³⁺ was found to be very impactful toward an efficient water oxidation mechanism. Certainly, the Jahn–Teller distortion associated with the low-spin electronic configuration instigates a defect center often known to be an active center leading to surface reconstruction beneficial for OER activity. The electrocatalyst exhibited an outstanding OER activity with an ultralow overpotential of 216 mV to achieve a 20 mA cm^–2 current density and a lower Tafel slope value of 50 mV dec^–1 in alkaline media. The ability of the electrocatalyst was further explored toward seawater oxidation, demonstrating it to be a potential candidate with an outstanding durability of over 160 h at a high current density of 500 mA cm^–2 in alkaline real seawater.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142188127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interfacial Distribution Effects of Potassium Fluoride on Enhancing Performance and UV Stability of Perovskite Solar Cells","authors":"Hui Wang,&nbsp;Likun Wang,&nbsp;Tianqi Niu*,&nbsp;Wenli Shang,&nbsp;Xiaochun Zhang,&nbsp;Zhenghui Wan,&nbsp;Xin Chen,&nbsp;Weidong Zhu,&nbsp;Kai Wang*,&nbsp;Shengzhong Frank Liu and Chunfu Zhang*,&nbsp;","doi":"10.1021/acsaem.4c0197510.1021/acsaem.4c01975","DOIUrl":"https://doi.org/10.1021/acsaem.4c01975https://doi.org/10.1021/acsaem.4c01975","url":null,"abstract":"<p >Perovskite photovoltaics offer a promising solution for lightweight power generation for near-space applications. The key factors including device efficiency and long-term ultraviolet (UV) light stability are essential for ensuring the sustainability of energy harvesting devices, yet to be further improved for perovskite solar cells (PSCs). In this work, a synergetic interface modification strategy, utilizing potassium fluoride (KF) as the modifier in SnO₂, was developed to passivate charged defects and regulate the electronic properties at the KF-SnO₂/perovskite interface. The optimization impacts of KF were systematically revealed by examining the spatial distribution of its binary ionic components and related coordination effects at the contact interface. The K⁺ ions can migrate into the bulk perovskite serve to passivate the grain boundaries and stabilize the lattice structure, while F^– ions prefer to retain within the SnO₂ layer to tailor the interfacial properties. The KF modification collectively contributes to significant improvements in defect passivation, energetic alignment, suppression of nonradiative recombination, and UV resistance of PSCs. As a result, the KF-SnO₂-based PSCs achieved an efficiency of 23.17%, retaining more than 90% of the original efficiency after over 1000 h of continuous UV-light illumination or 350 h of operation under one sun illumination. Furthermore, we validated the compatibility of KF-SnO₂ in the scalable fabrication process, demonstrating that 8 × 4 cm² flexible perovskite solar modules (active area of 26.0 cm²) achieved an efficiency of 14.26%. This highlights the benefits of KF-based interface engineering for advancing the upscaling and high-performance PSCs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}