ACS Energy Letters 最新文献_第10页

An Amphiphilic Proton Donor Decouples Acidity from Interfacial Reactivity for Lithium-Mediated Ammonia Synthesis 一种两亲性质子供体将酸性从锂介导的氨合成的界面反应活性中解耦

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-07 DOI: 10.1021/acsenergylett.6c02477

Yeongbae Jeon,Shihyun Kim,Seong Hyeon Kweon,Bongseok Kim,Ahee Choi,Hyun Ji An,Seungwon Chung,Dongjun Kim,Sang Kyu Kwak,Jungwon Park,Yun Jeong Hwang

{"title":"An Amphiphilic Proton Donor Decouples Acidity from Interfacial Reactivity for Lithium-Mediated Ammonia Synthesis","authors":"Yeongbae Jeon,Shihyun Kim,Seong Hyeon Kweon,Bongseok Kim,Ahee Choi,Hyun Ji An,Seungwon Chung,Dongjun Kim,Sang Kyu Kwak,Jungwon Park,Yun Jeong Hwang","doi":"10.1021/acsenergylett.6c02477","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02477","url":null,"abstract":"Abstract Electrochemical ammonia synthesis via a lithium-mediated nitrogen reduction reaction (Li-NRR) faces a fundamental selectivity challenge in which proton donors that accelerate productive protonation simultaneously promote parasitic hydrogen evolution. Here, we demonstrate that 2,2,2-trifluoroethanol (TFE), an amphiphilic alcohol, mitigates this limitation by decoupling thermodynamic acidity from kinetic reactivity. Despite its high acidity, TFE suppresses parasitic reactions through rapid interfacial passivation associated with its fluorinated structure, while modulating the microstructure of a fluoride-rich solid electrolyte interphase (SEI). Blending TFE with ethanol further optimizes proton activity and hydrogen bonding, yielding a thin, uniform SEI enriched in highly crystalline LiF with reduced interfacial resistance. The optimized electrolyte achieved a Faradaic efficiency of 59.0% in a continuous-flow reactor, maintained stable performance under potential-cycling, and reached 82.8% in a high-pressure batch reactor. This study highlights proton-donor engineering as a key strategy to modulate the SEI nanostructure for selectivity in Li-NRR.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"59 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Suppressing 2D Interfacial Reconstruction via Tetrafluoroborate Surface Engineering for Stable Perovskite Solar Cells 稳定钙钛矿太阳能电池的四氟硼酸盐表面工程抑制二维界面重建

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-07 DOI: 10.1021/acsenergylett.6c01987

Sanjay Sandhu,Zhenghong Xiong,Xin Liang,Nam-Gyu Park

{"title":"Suppressing 2D Interfacial Reconstruction via Tetrafluoroborate Surface Engineering for Stable Perovskite Solar Cells","authors":"Sanjay Sandhu,Zhenghong Xiong,Xin Liang,Nam-Gyu Park","doi":"10.1021/acsenergylett.6c01987","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01987","url":null,"abstract":"Abstract Surface passivation using two-dimensional (2D) perovskites has been widely employed to improve the efficiency and stability of perovskite solar cells (PSCs). However, conventional 3D/2D heterointerfaces often suffer from interfacial reconstruction caused by spacer-cation migration during operation, leading to performance degradation. Here, we investigate pseudo-halogen-modified phenethylammonium salts (PEAX, X = SCN and BF4) for surface passivation. Unlike the commonly used phenethylammonium iodide (PEAI), which forms a low-dimensional interfacial phase, PEABF4 does not induce 2D perovskite formation but instead enables non-reconstructive surface passivation. PEABF4 treatment improves energy-level alignment, carrier lifetime, charge extraction, and crystallinity and suppresses surface traps and nonradiative recombination. As a result, PSCs achieve a power conversion efficiency of 24.72% with a VOC of 1.16 V, outperforming untreated and PEAI-treated devices. Furthermore, unencapsulated PEABF4-based devices retain 85.96% of their initial efficiency after 320 h of maximum power point tracking, demonstrating that pseudo-halogen engineering offers an effective route toward efficient and operationally stable PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thermodynamic Control of Excitation Transport Regimes in Nanocrystal Solids 纳米晶体固体中激发输运机制的热力学控制

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02596

Thomas B. Haward,Vincent J.-Y. Lim,Ihor Cherniukh,Joshua R. S. Lilly,Adam T. M. Wood,Maryna I. Bodnarchuk,Michael B. Johnston,Maksym V. Kovalenko,Laura M. Herz

{"title":"Thermodynamic Control of Excitation Transport Regimes in Nanocrystal Solids","authors":"Thomas B. Haward,Vincent J.-Y. Lim,Ihor Cherniukh,Joshua R. S. Lilly,Adam T. M. Wood,Maryna I. Bodnarchuk,Michael B. Johnston,Maksym V. Kovalenko,Laura M. Herz","doi":"10.1021/acsenergylett.6c02596","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02596","url":null,"abstract":"Abstract Controlling excitation transport is central to the operation of light-harvesting and light-emitting devices based on nanocrystal films. Exciton diffusion is typically described as hopping through a homogeneous medium; however, even highly monodisperse nanocrystal ensembles exhibit energetic disorder arising from size variation. We demonstrate that such disorder couples exciton diffusivity in real space to energetic relaxation within the density of states. Using spectrally and temporally resolved photoluminescence reabsorption spectroscopy of CsPbBr3 nanocrystal films, we separately track exciton diffusion and energetic relaxation across a range of temperatures and nanocrystal sizes. We find that at low temperature, excitons preferentially migrate downhill toward larger, lower-energy nanocrystals, causing a transient collapse of exciton diffusivity that is particularly pronounced for smaller nanocrystals exhibiting higher energetic disorder. At room temperature, these effects are effectively countered by thermally activated uphill transfer, restoring normal diffusion. Nanocrystal solids thus offer tunable transport properties governed by the interplay between disorder and thermal energy.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"2 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dynamic Solvent Participation Drives Sodium Storage in Oxygen Engineered Hard Carbon 动态溶剂参与驱动氧工程硬碳中钠的储存

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02029

Jian Cui,Panpan Su,Jie Zhang,Ruiyi Li,Zuoyi Xiao,Qingda An,Zhongwei Chen

引用次数: 0

Humidity-Regulated Wetting of Aqueous PEDOT:PSS Enables Surfactant-Free Hole-Transport Layers in Non-Fullerene-Based Inverted Organic Photovoltaics 水分PEDOT的湿度调节润湿：PSS在非富勒烯基倒置有机光伏中实现无表面活性剂的空穴传输层

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02028

Karin Iwa,Lulu Sun,Kazuma Nakajima,Ryota Fukuzawa,Shinjiro Umezu,Thuc-Quyen Nguyen,Daishi Inoue,Daisuke Hashizume,Sunghoon Lee,Kenjiro Fukuda,Takao Someya

{"title":"Humidity-Regulated Wetting of Aqueous PEDOT:PSS Enables Surfactant-Free Hole-Transport Layers in Non-Fullerene-Based Inverted Organic Photovoltaics","authors":"Karin Iwa,Lulu Sun,Kazuma Nakajima,Ryota Fukuzawa,Shinjiro Umezu,Thuc-Quyen Nguyen,Daishi Inoue,Daisuke Hashizume,Sunghoon Lee,Kenjiro Fukuda,Takao Someya","doi":"10.1021/acsenergylett.6c02028","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02028","url":null,"abstract":"Abstract Inverted organic photovoltaics (OPVs) feature operational stability; however, developing fully solution-processed devices remains challenging due to the poor wettability of PEDOT:PSS hole-transport layers (HTLs) on hydrophobic donor:acceptor bulk heterojunction active layers. Here, we demonstrate a surfactant-free, humidity-regulated spin-coating strategy for forming uniform PEDOT:PSS HTLs directly on PM6:Y6 active layers. By maintaining the relative humidity at 10% or lower during coating, continuous PEDOT:PSS films were obtained, enabling inverted OPVs with power conversion efficiency (PCE) above 14.5%. Furthermore, these devices retain over twice the PCE of molybdenum oxide-based devices after 100 h of light soaking under nitrogen. Bulk quantum efficiency analysis suggests that the acidic aqueous PEDOT:PSS dispersion may partially perturb the interface on the active layer, whereas it improves the overall device stability. This humidity-regulated coating approach provides a simple route toward solution-processable HTL integration in efficient and operationally stable inverted OPVs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"54 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Passivation Suppresses α-Particle-Induced Trap Formation in Perovskite Solar Cells for Space Applications 空间应用钙钛矿太阳能电池表面钝化抑制α-粒子诱导的陷阱形成

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-05 DOI: 10.1021/acsenergylett.6c02610

Da Seul Lee,Hyeong Won Seo,Hyeji Han,Suwhan Kim,Suseong Jang,Sang Won Kang,Sungwon Cho,Seung Hyeon Chae,Donghan Kang,Nayeong Kwon,Nuri Na,Dong-Won Kang,Dohyung Kim,Jongchul Lim,Dong-Seok Kim,Jongsung Park

{"title":"Surface Passivation Suppresses α-Particle-Induced Trap Formation in Perovskite Solar Cells for Space Applications","authors":"Da Seul Lee,Hyeong Won Seo,Hyeji Han,Suwhan Kim,Suseong Jang,Sang Won Kang,Sungwon Cho,Seung Hyeon Chae,Donghan Kang,Nayeong Kwon,Nuri Na,Dong-Won Kang,Dohyung Kim,Jongchul Lim,Dong-Seok Kim,Jongsung Park","doi":"10.1021/acsenergylett.6c02610","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02610","url":null,"abstract":"Abstract α-Particles represent the second most abundant ionic species in space radiation, yet their specific degradation mechanisms and mitigation strategies in perovskite solar cells (PSCs) remain unquantified. Here, we evaluate the degradation of PSCs under 2.5 MeV α-particle irradiation and investigate the protective role of a propane-1,3-diammonium iodide (PDAI2) surface passivation. Following irradiation, PDAI2-passivated target devices retain 80% of their initial efficiency (20.22%), whereas control devices retain 60% (19.13%). Performance losses were dominated by fill factor degradation. X-ray diffraction, scanning electron microscopy, and Fourier-transform infrared spectroscopy indicate that while α-particle induces partial organic cation loss and morphological variations, the primary crystalline phase is preserved without secondary phase decomposition. Capacitance–voltage, impedance spectroscopy, and Kelvin probe force microscopy confirmed that performance losses originate predominantly from photoactive trap states generated at the perovskite surface and interface, which increase space-charge density and transport resistance. Diammonium cations coordinate undercoordinated surface sites and crosslink organic cations, preventing radiation-generated point defects from stabilizing into transport-impeding traps. These findings establish surface defect chemistry control as a key strategy against high linear energy transfer (LET) ion radiation in space photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Wireless Monolithic Tandem Leaf for Semi-Artificial Photosynthesis 半人工光合作用的无线单片串联叶片

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-05 DOI: 10.1021/acsenergylett.6c01999

Minah Kim,Jihong Min,Chang Hyun Kim,Hyun-Woo Kim,Donggu Kim,Yire Han,Yonghoon Jung,Hanseul Choi,Hoyoung Song,Hyewon Park,Soo-Jin Yeom,Kwanyong Seo,Yun Seog Lee,Yoonmook Kang,Jeong Young Park,Byungha Shin,Chan Beum Park

{"title":"Wireless Monolithic Tandem Leaf for Semi-Artificial Photosynthesis","authors":"Minah Kim,Jihong Min,Chang Hyun Kim,Hyun-Woo Kim,Donggu Kim,Yire Han,Yonghoon Jung,Hanseul Choi,Hoyoung Song,Hyewon Park,Soo-Jin Yeom,Kwanyong Seo,Yun Seog Lee,Yoonmook Kang,Jeong Young Park,Byungha Shin,Chan Beum Park","doi":"10.1021/acsenergylett.6c01999","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01999","url":null,"abstract":"Abstract Biocatalytic semi-artificial photosynthesis enables selective solar-to-chemical conversion by harnessing photoelectrocatalytic platforms to drive redox biocatalysis. However, the reliance of most photoelectrochemical (PEC)-based devices on transparent conductive oxides (TCOs) or wired configurations introduces resistive losses and architectural complexity, limiting the translation of biosolar conversion beyond laboratory-scale systems. Here, we report a wireless, monolithic semi-artificial leaf device toward scalable and practical solar biosynthesis. The PEC tandem, composed of a poly(ethylene glycol) (PEG)-modified BiVO4 (PEG:BiVO4) photoanode and a tunnel-oxide-passivated-contact (TOPCon) Si photovoltaic (PV), supplies sufficient photovoltage to reduce O2 to H2O2 on an anthraquinone-2-carboxylic acid (AQC)-functionalized carbon-fiber paper (CFP) cathode under solar light, sustaining over 100 h of stable operation. The photogenerated H2O2 reacts with peroxygenases to catalyze the oxyfunctionalization of substituted benzenes, alkanes, and fatty acids with record-high total turnover numbers of 166,100 (unspecific peroxygenase) and 3,700 (cytochrome P450). Furthermore, the scaling of the PEC device allows the direct conversion of natural light into enantiopure alcohols.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091724","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Asymmetric Ion Regulation for Stabilising Acidic CO2 Electrolysis and Chlorine Evolution in Zero-Gap Electrolysers 零间隙电解槽中稳定酸性CO2电解和氯析出的不对称离子调控

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-04 DOI: 10.1021/acsenergylett.6c02502

Zehua Wang,Yong Zhao,Chaochen Xu,Changya Deng,Zhixin Luo,Zhiliang Wu,Zongping Shao,Tejas Bhatelia,Sahil Garg

{"title":"Asymmetric Ion Regulation for Stabilising Acidic CO2 Electrolysis and Chlorine Evolution in Zero-Gap Electrolysers","authors":"Zehua Wang,Yong Zhao,Chaochen Xu,Changya Deng,Zhixin Luo,Zhiliang Wu,Zongping Shao,Tejas Bhatelia,Sahil Garg","doi":"10.1021/acsenergylett.6c02502","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02502","url":null,"abstract":"Abstract While CO2 reduction reaction (CO2RR) coupled with chlorine evolution reaction (CER) can enhance the energy efficiency and economic viability of CO2 electrolysis, its implementation in zero-gap membrane-electrode-assembly (MEA) electrolysers remains challenging as CER-compatible systems require acidic chloride-rich anolytes and chlorine-tolerant cation exchange membranes that induce detrimental cation crossover. The resulting disruption of the cathodic microenvironment causes (bi)carbonate precipitation, hydrogen evolution, and operational instability. Here we report an asymmetric ion-regulation strategy using chloride-bearing, water-miscible poly(diallyldimethylammonium chloride) in the anolyte to maintain high chloride availability for CER while reducing K+ crossover and modifying proton transport through the membrane. Optimised MEA electrolysers achieve about 90% Faradaic efficiencies for both CO and Cl2 and more than 200 h of cumulative operation under replenishment/maintenance protocols, advancing CO2RR-CER beyond laboratory flow-cell demonstrations toward zero-gap MEA operation. Techno-economic and life-cycle analyses indicate that Cl2 co-production can improve process economics under the stated assumptions and reduce the greenhouse-gas intensity of CO production by 75% relative to conventional CO2RR coupled with oxygen evolution benchmarks.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Hybrid Phosphate–Ether Electrolyte for High-Temperature and High-Safety 18650 Cylindrical Sodium-Ion Batteries 用于高温高安全18650圆柱钠离子电池的磷酸盐-醚混合电解质

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-02 DOI: 10.1021/acsenergylett.6c02299

Zhiming Zhou,Guojun Yu,Yun Gao,Hang Zhang,Xingqiao Wu,Xiaohao Liu,Li Li,Lin Li,Shulei Chou

引用次数: 0

Understanding the Role of Lithium Metal Microstructure in Chemo-Mechanical Instability of Solid-State Batteries 金属锂微观结构在固态电池化学-机械不稳定性中的作用

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-02 DOI: 10.1021/acsenergylett.6c02372

Deep Chatterjee,Abhinand Ayyaswamy,Bairav S. Vishnugopi,Jeong Seop Yoon,Donald J. Siegel,Jeff Sakamoto,Partha P. Mukherjee

{"title":"Understanding the Role of Lithium Metal Microstructure in Chemo-Mechanical Instability of Solid-State Batteries","authors":"Deep Chatterjee,Abhinand Ayyaswamy,Bairav S. Vishnugopi,Jeong Seop Yoon,Donald J. Siegel,Jeff Sakamoto,Partha P. Mukherjee","doi":"10.1021/acsenergylett.6c02372","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02372","url":null,"abstract":"Abstract Increased energy density and safety relative to conventional lithium (Li)-ion batteries motivate the development of solid-state batteries (SSBs). However, maintaining interface stability at the metal anode–solid electrolyte (SE) interface remains a critical challenge to achieving practical areal capacities, especially during stripping/discharge. Here, a mesoscale model informed by atomistic simulations is employed to examine void formation at the Li metal–SE interface during discharge/stripping. The model reveals how void-formation-driven interfacial contact loss behavior depends on the microstructural properties of the polycrystalline Li anode. In agreement with prior studies, Li microstructures with small grain sizes promote self-diffusion-induced void healing and generally exhibit better interfacial contact. We further show the effect of operating conditions, such as applied pressure, stripping current density, and temperature, on the stripping performance for different Li microstructures. Through this study, we shed light on the importance of taking microstructural features into account in predicting interfacial contact evolution during stripping of Li metal SSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"295 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0