ACS Energy Letters Pub Date : 2025-01-15DOI: 10.1021/acsenergylett.4c0351510.1021/acsenergylett.4c03515
Desui Chen, Bing Tang, Aleksandr A. Sergeev, Ye Wu, Haochen Liu, Ding Zhu, Sile Hu, Kam Sing Wong, Hin-Lap Yip* and Andrey L. Rogach*,
{"title":"Green Spin Light-Emitting Diodes Enabled by Perovskite Nanocrystals in Situ Modified with Chiral Ligands","authors":"Desui Chen, Bing Tang, Aleksandr A. Sergeev, Ye Wu, Haochen Liu, Ding Zhu, Sile Hu, Kam Sing Wong, Hin-Lap Yip* and Andrey L. Rogach*, ","doi":"10.1021/acsenergylett.4c0351510.1021/acsenergylett.4c03515","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03515https://doi.org/10.1021/acsenergylett.4c03515","url":null,"abstract":"<p >Spin-polarized light-emitting diodes (spin-LEDs) hold promise for next-generation technologies across optical communication, biological imaging, and quantum information processing. Chiral metal halide perovskites, which combine advantageous optoelectronic properties with chirality, are promising materials for high-performance spin-LEDs. However, such spin-LEDs still suffer from low efficiency and limited brightness, as they often rely on low-dimensional chiral perovskites with rather inferior charge-transport properties as spin filter layers. Herein, we demonstrate bright and efficient green spin-LEDs based on chiral perovskite nanocrystals as emitters. We employed an <i>in situ</i> chiral ligand modification using R-/S-1-(4-bromophenyl)-ethylammonium bromide to imprint chirality onto CsPbBr<sub>3</sub> nanocrystals, which exhibited both a high photoluminescence quantum yield of 89% and improved spin relaxation lifetime. A remarkable spin-polarization of 88% was observed for the CsPbBr<sub>3</sub> nanocrystal films. Consequently, our spin-LEDs without a commonly used spin filter layer simultaneously achieved a maximum brightness of 12,800 cd m<sup>–2</sup>, a record-high peak external quantum efficiency of 15.4%, and a circularly polarized electroluminescence with a dissymmetry factor of 2.16 × 10<sup>–3</sup> at room temperature, setting new benchmarks for perovskite-based spin-LEDs.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"815–821 815–821"},"PeriodicalIF":19.3,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c03515","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Desui Chen, Bing Tang, Aleksandr A. Sergeev, Ye Wu, Haochen Liu, Ding Zhu, Sile Hu, Kam Sing Wong, Hin-Lap Yip, Andrey L. Rogach
{"title":"Green Spin Light-Emitting Diodes Enabled by Perovskite Nanocrystals in Situ Modified with Chiral Ligands","authors":"Desui Chen, Bing Tang, Aleksandr A. Sergeev, Ye Wu, Haochen Liu, Ding Zhu, Sile Hu, Kam Sing Wong, Hin-Lap Yip, Andrey L. Rogach","doi":"10.1021/acsenergylett.4c03515","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03515","url":null,"abstract":"Spin-polarized light-emitting diodes (spin-LEDs) hold promise for next-generation technologies across optical communication, biological imaging, and quantum information processing. Chiral metal halide perovskites, which combine advantageous optoelectronic properties with chirality, are promising materials for high-performance spin-LEDs. However, such spin-LEDs still suffer from low efficiency and limited brightness, as they often rely on low-dimensional chiral perovskites with rather inferior charge-transport properties as spin filter layers. Herein, we demonstrate bright and efficient green spin-LEDs based on chiral perovskite nanocrystals as emitters. We employed an <i>in situ</i> chiral ligand modification using R-/S-1-(4-bromophenyl)-ethylammonium bromide to imprint chirality onto CsPbBr<sub>3</sub> nanocrystals, which exhibited both a high photoluminescence quantum yield of 89% and improved spin relaxation lifetime. A remarkable spin-polarization of 88% was observed for the CsPbBr<sub>3</sub> nanocrystal films. Consequently, our spin-LEDs without a commonly used spin filter layer simultaneously achieved a maximum brightness of 12,800 cd m<sup>–2</sup>, a record-high peak external quantum efficiency of 15.4%, and a circularly polarized electroluminescence with a dissymmetry factor of 2.16 × 10<sup>–3</sup> at room temperature, setting new benchmarks for perovskite-based spin-LEDs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981273","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}
ACS Energy Letters Pub Date : 2025-01-15DOI: 10.1021/acsenergylett.4c0309110.1021/acsenergylett.4c03091
Tae-Ung Wi, Zachary H Levell, Shaoyun Hao, Ahmad Elgazzar, Peng Zhu, Yuge Feng, Feng-Yang Chen, Wei Ping Lam, Mohsen Shakouri, Yuanyue Liu* and Haotian Wang*,
{"title":"Selective and Stable Ethanol Synthesis via Electrochemical CO2 Reduction in a Solid Electrolyte Reactor","authors":"Tae-Ung Wi, Zachary H Levell, Shaoyun Hao, Ahmad Elgazzar, Peng Zhu, Yuge Feng, Feng-Yang Chen, Wei Ping Lam, Mohsen Shakouri, Yuanyue Liu* and Haotian Wang*, ","doi":"10.1021/acsenergylett.4c0309110.1021/acsenergylett.4c03091","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03091https://doi.org/10.1021/acsenergylett.4c03091","url":null,"abstract":"<p >Electrochemical CO<sub>2</sub> reduction to ethanol faces challenges such as low selectivity, a product mixture with liquid electrolyte, and poor catalyst/reactor stability. Here, we developed a grain-rich zinc-doped Cu<sub>2</sub>O precatalyst that presented a high ethanol Faradaic efficiency of over 40% under a current density of 350 mA·cm<sup>–2</sup>. Our density functional theory (DFT) simulation suggested that Zn atoms inside the structure have a greater carbophilicity than the Cu atoms to help facilitate *CHCHO formation, a key reaction intermediate toward ethanol instead of other C<sub>2</sub> products. A high Faradaic efficiency ratio between ethanol and ethylene (FE<sub>EtOH</sub>/FE<sub>C2H4</sub>) reached 2.34 in the zinc-doped Cu<sub>2</sub>O precatalyst, representing an over 4-fold improvement compared to bare Cu<sub>2</sub>O precatalyst. By integrating this Cu-based catalyst into a porous solid electrolyte (PSE) reactor with a salt-managing design, we achieved stable ethanol production for over 180 h under a current density of 250 mA·cm<sup>–2</sup> while maintaining ethanol selectivity at ∼30%.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"822–829 822–829"},"PeriodicalIF":19.3,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402060","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}
Yalan Zhang, Tinghuan Yang, Sang-Uk Lee, Shengzhong Liu, Kui Zhao, Nam-Gyu Park
{"title":"Correction to “Stabilizing α-Phase FAPbI3 Perovskite Induced by an Ordered Solvated Quasi-Crystalline PbI2”","authors":"Yalan Zhang, Tinghuan Yang, Sang-Uk Lee, Shengzhong Liu, Kui Zhao, Nam-Gyu Park","doi":"10.1021/acsenergylett.4c03542","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03542","url":null,"abstract":"In Figure S18 in the Supporting Information, the colors for control and target samples were mistakenly displayed. The updated figure is below. The paragraph explaining Figure S18 was correctly described in the original manuscript, as “The <i>E</i><sub>a</sub> of the target device is 201 meV, which is two times higher than that of the control device (100 meV).” The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.4c03542. Additional experimental results and data (Figures S1–S18 and Tables S1–S7), including statistical performance parameters, XRD patterns, AFM images, UPS spectra, EQE spectra, thermal stability, Nyquist plots, transient photocurrent decay measurements, and temperature-dependent conductivity measurements (PDF) Correction to “Stabilizing α‑Phase\u0000FAPbI<sub>3</sub> Perovskite Induced by an Ordered Solvated Quasi-Crystalline\u0000PbI<sub>2</sub>” <span> 0 </span><span> views </span> <span> 0 </span><span> shares </span> <span> 0 </span><span> downloads </span> Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. This article has not yet been cited by other publications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981274","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}
Xitao Lin, Jing Zhou, Jing Liu, Xu Li, Yanan Zhao, Min Jia, Tiehan Mei, Jin Ye, Maowen Xu, Yubin Niu
{"title":"Electronic Structure Modulation Enables Sodium Compensation in Cathode Organic Additives for Sodium-Ion Batteries","authors":"Xitao Lin, Jing Zhou, Jing Liu, Xu Li, Yanan Zhao, Min Jia, Tiehan Mei, Jin Ye, Maowen Xu, Yubin Niu","doi":"10.1021/acsenergylett.4c03323","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03323","url":null,"abstract":"To address the issue of reduced energy density in sodium-ion full cells due to irreversible sodium ion losses, the cathode sodium compensation additive method is the usual approach nowadays; however, finding efficient, low-voltage, and low-cost additives remains a challenge. This work develops a class of organic additives, i.e., N-substituted main-chain C organic compounds. Compared with all-C or O-substituted organics, the N-substituted organics show lower decomposition potentials due to the stronger electron-donating effect of N, and the potentials will be further reduced if other electron-donating groups are introduced. When introduced as an additive into a P2–Na<sub>2/3</sub>Ni<sub>1/3</sub>Mn<sub>1/3</sub>Ti<sub>1/3</sub>O<sub>2</sub> cathode, an addition of 10 wt % enhances the initial charging capacity from 96.3 to 189.4 mAh g<sup>–1</sup> and does not cause cycling or rate capability deterioration. The full cells paired with hard carbon anode exhibit higher energy densities (150.6 vs 235.1 Wh kg<sup>–1</sup>), suggesting that such additives offer great potential for practical applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981172","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}
Jingchen Na, Hongmei Yu, Jun Chi, Senyuan Jia, Zhigang Shao
{"title":"Operando Electrochemical Reduction Reconstruction Boosted Long-Term Overall Seawater Splitting","authors":"Jingchen Na, Hongmei Yu, Jun Chi, Senyuan Jia, Zhigang Shao","doi":"10.1021/acsenergylett.4c03209","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03209","url":null,"abstract":"Seawater electrolysis technology utilizes surplus renewable energy from maritime and coastal stations. However, the aggressive Cl<sup>–</sup> in seawater caused the anodic kinetic restraints and metal dissolution deactivation, restricting the efficiency and durability of seawater electrolyzers. In this study, a convenient optimizing/retrieving strategy of the operando electrochemical reduction reconstruction (RR) has been proposed to reclaim the dissolved Fe ions from NiFe Foam by electrodeposition and decorate it onto the catalyst surface with the formation of electrophilic FeOOH. The operando electrochemistry techniques revealed that the RR-anchored FeOOH facilitated the anodic reorganization of amorphous γ-NiOOH, thus inhibiting chloride poisoning and boosting seawater oxygen evolution. Hence, the RR-optimized NiCoS NAs/NFF || NiCoS NAs/NFF showed a performance elevation (−265.4 μV h<sup>–1</sup>) over 500 h of overall natural seawater splitting at 600 mA cm<sup>–2</sup> enabled by these strategic approaches. This investigation provided insight into the utilization of dissolved metal during overall seawater splitting and exhibited a promising future for long-term efficient electrolysis under harsh conditions.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"209 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142974759","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}
Jasper Biemolt, Jai Singh, Gerard Prats Vergel, Henri M. Pelzer, Thomas Burdyny
{"title":"Preventing Salt Formation in Zero-Gap CO2 Electrolyzers by Quantifying Cation Accumulation","authors":"Jasper Biemolt, Jai Singh, Gerard Prats Vergel, Henri M. Pelzer, Thomas Burdyny","doi":"10.1021/acsenergylett.4c03242","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03242","url":null,"abstract":"The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) in a membrane electrode assembly (MEA) efficiently turns CO<sub>2</sub> into a feedstock. However, unfavorable steady-state concentrations of ions in the cathode compartment result in salt formation if unaddressed, which restricts the access of CO<sub>2</sub> and causes cell failure. Here, we systematically show the relationship between salt accumulation and four system parameters including cation species, anolyte concentration, membrane thickness, and operating temperature. To compare each metric, we quantified the cation accumulation rate at predefined operating times. Notably, we show that operating at temperatures above 50 °C with properly humidified CO<sub>2</sub> stream fully avoids salt formation. We further show that combining separate operating conditions is also highly effective, showing operation for >144 h with no measurable salt deposition at 200 mA/cm<sup>2</sup>. Collectively, our work systematically demonstrates that salt formation is a prevalent yet surmountable CO<sub>2</sub>RR challenge that can be overcome by elevated cell temperatures or switching to more soluble alkali cations.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"42 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981275","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}
ACS Energy Letters Pub Date : 2025-01-14DOI: 10.1021/acsenergylett.4c0320910.1021/acsenergylett.4c03209
Jingchen Na, Hongmei Yu*, Jun Chi, Senyuan Jia and Zhigang Shao*,
{"title":"Operando Electrochemical Reduction Reconstruction Boosted Long-Term Overall Seawater Splitting","authors":"Jingchen Na, Hongmei Yu*, Jun Chi, Senyuan Jia and Zhigang Shao*, ","doi":"10.1021/acsenergylett.4c0320910.1021/acsenergylett.4c03209","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03209https://doi.org/10.1021/acsenergylett.4c03209","url":null,"abstract":"<p >Seawater electrolysis technology utilizes surplus renewable energy from maritime and coastal stations. However, the aggressive Cl<sup>–</sup> in seawater caused the anodic kinetic restraints and metal dissolution deactivation, restricting the efficiency and durability of seawater electrolyzers. In this study, a convenient optimizing/retrieving strategy of the operando electrochemical reduction reconstruction (RR) has been proposed to reclaim the dissolved Fe ions from NiFe Foam by electrodeposition and decorate it onto the catalyst surface with the formation of electrophilic FeOOH. The operando electrochemistry techniques revealed that the RR-anchored FeOOH facilitated the anodic reorganization of amorphous γ-NiOOH, thus inhibiting chloride poisoning and boosting seawater oxygen evolution. Hence, the RR-optimized NiCoS NAs/NFF || NiCoS NAs/NFF showed a performance elevation (−265.4 μV h<sup>–1</sup>) over 500 h of overall natural seawater splitting at 600 mA cm<sup>–2</sup> enabled by these strategic approaches. This investigation provided insight into the utilization of dissolved metal during overall seawater splitting and exhibited a promising future for long-term efficient electrolysis under harsh conditions.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"788–797 788–797"},"PeriodicalIF":19.3,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402462","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}
ACS Energy Letters Pub Date : 2025-01-14DOI: 10.1021/acsenergylett.4c0324210.1021/acsenergylett.4c03242
Jasper Biemolt, Jai Singh, Gerard Prats Vergel, Henri M. Pelzer and Thomas Burdyny*,
{"title":"Preventing Salt Formation in Zero-Gap CO2 Electrolyzers by Quantifying Cation Accumulation","authors":"Jasper Biemolt, Jai Singh, Gerard Prats Vergel, Henri M. Pelzer and Thomas Burdyny*, ","doi":"10.1021/acsenergylett.4c0324210.1021/acsenergylett.4c03242","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03242https://doi.org/10.1021/acsenergylett.4c03242","url":null,"abstract":"<p >The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) in a membrane electrode assembly (MEA) efficiently turns CO<sub>2</sub> into a feedstock. However, unfavorable steady-state concentrations of ions in the cathode compartment result in salt formation if unaddressed, which restricts the access of CO<sub>2</sub> and causes cell failure. Here, we systematically show the relationship between salt accumulation and four system parameters including cation species, anolyte concentration, membrane thickness, and operating temperature. To compare each metric, we quantified the cation accumulation rate at predefined operating times. Notably, we show that operating at temperatures above 50 °C with properly humidified CO<sub>2</sub> stream fully avoids salt formation. We further show that combining separate operating conditions is also highly effective, showing operation for >144 h with no measurable salt deposition at 200 mA/cm<sup>2</sup>. Collectively, our work systematically demonstrates that salt formation is a prevalent yet surmountable CO<sub>2</sub>RR challenge that can be overcome by elevated cell temperatures or switching to more soluble alkali cations.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"807–814 807–814"},"PeriodicalIF":19.3,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c03242","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}