Chun Wang (, ), Yang Liu (, ), Renlong Zhu (, ), Tianpei Zhou (, ), Minghao Wang (, ), Han Cheng (, ), Wenjie Wang (, ), Xiaolin Tai (, ), Lin Wang (, ), Long Chen (, ), Yue Lin (, ), Shuji Ye (, ), Yi Xie (, ), Changzheng Wu (, )
{"title":"New layered organic-inorganic superlattice with bilayer linear molecules for superhigh heat insulation","authors":"Chun Wang \u0000 (, ), Yang Liu \u0000 (, ), Renlong Zhu \u0000 (, ), Tianpei Zhou \u0000 (, ), Minghao Wang \u0000 (, ), Han Cheng \u0000 (, ), Wenjie Wang \u0000 (, ), Xiaolin Tai \u0000 (, ), Lin Wang \u0000 (, ), Long Chen \u0000 (, ), Yue Lin \u0000 (, ), Shuji Ye \u0000 (, ), Yi Xie \u0000 (, ), Changzheng Wu \u0000 (, )","doi":"10.1007/s40843-024-3102-y","DOIUrl":"10.1007/s40843-024-3102-y","url":null,"abstract":"<div><p>Layered inorganic materials provide an essential platform for constructing new structural configurations of materials with exceptional properties. However, precise control over the interlayer molecular arrangement remains a significant challenge, impeding in-depth exploration in physics and chemistry realm. Herein, we demonstrated a new layered organic-inorganic superlattice composed of a S-Ta-S inorganic lattice and bilayer linear molecules, providing superhigh heat insulation. A series of interlayer-confined intercalations of alkylamines with increasing chain length in the layered inorganic materials were achieved through precisely ordered molecule design (TaS<sub>2</sub>-C<i>n</i>, <i>n</i> = 3, 6, 8, 12). Systematic spectral analysis reveals that as the length of the intercalated alkyl chain increases, the alkyl chain between layers becomes more ordered and linear, and the gauche conformation decreases. Furthermore, the more linear and ordered alkyl chain conformation results in lower thermal conductivity. The thermal conductivity of TaS<sub>2</sub>-C12 is 0.426 W m<sup>−1</sup> K<sup>−1</sup>, which is only one-third that of the pristine TaS<sub>2</sub> crystal. We anticipate that this layered organic-inorganic superlattice design will pave a new avenue for developing new organic-inorganic functional materials and probing the limits of ultralow thermal conductivity materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 12","pages":"4065 - 4073"},"PeriodicalIF":6.8,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yunna Guo (, ), Hantao Cui (, ), Zhangran Ye (, ), Xixi Qin (, ), Peng Jia (, ), Lei Deng (, ), Chongchong Ma (, ), Chao Tai (, ), Liqiang Zhang (, ), Bin Wen (, )
{"title":"Atomic processing of two-dimensional amorphous carbon","authors":"Yunna Guo \u0000 (, ), Hantao Cui \u0000 (, ), Zhangran Ye \u0000 (, ), Xixi Qin \u0000 (, ), Peng Jia \u0000 (, ), Lei Deng \u0000 (, ), Chongchong Ma \u0000 (, ), Chao Tai \u0000 (, ), Liqiang Zhang \u0000 (, ), Bin Wen \u0000 (, )","doi":"10.1007/s40843-024-3100-9","DOIUrl":"10.1007/s40843-024-3100-9","url":null,"abstract":"<div><p>Two-dimensional amorphous carbon (2DAC) materials possess characteristics such as high conductivity, high flexibility, and chemical stability, making them promising for applications in electronics, sensors, catalysts, superconductors, energy storage, and energy conversion. However, it is still a challenge to directly synthesize 2DAC till now. Meanwhile, many controversies exist in their formation process and structure. Therefore, this article utilizes a top-down etching method to prepare 2DAC in environmental transmission electron microscope (ETEM). By employing electron beam irradiation combined with heating at 650°C in an oxygen atmosphere (0.01 mbar), controllable fabrication of 2DAC is achieved. In this process, the raw diamond sheet first transforms into graphite, and as the reaction goes on, the amount of graphite increases, eventually transitioning into 2DAC. First-principles calculations indicate that it is an energy-favorable process from diamond to graphite. Although there is an energy barrier for graphite-to-amorphous carbon transition, electron beam irradiation induces numerous defects that can overcome this barrier. This method not only fabricates 2DAC with atomic precision but also provides <i>in-situ</i> analysis of its formation process. The research findings contribute to a fundamental understanding of the formation process of 2DAC and offer new insights for the preparation of 2D ultrathin amorphous materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 12","pages":"4059 - 4064"},"PeriodicalIF":6.8,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Simultaneously achieving high sensitivity, low dark current and low detection limits in anti-perovskites towards X-ray detection","authors":"Haixing Meng, Ying Li","doi":"10.1007/s40843-024-3125-y","DOIUrl":"10.1007/s40843-024-3125-y","url":null,"abstract":"","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3757 - 3758"},"PeriodicalIF":6.8,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Stabilizing oxygen redox reaction in phase-transition-free P2-type Co/Ni-free cathode via Cu doping for sodium-ion batteries","authors":"Hai-Xia Zhang \u0000 (, ), Lin-Rong Wu \u0000 (, ), Hao-Rui Wang \u0000 (, ), Dong-Zheng Wu \u0000 (, ), Shao-Hui Guo \u0000 (, ), Ding Zhang \u0000 (, ), Xiao-Chuan Duan \u0000 (, ), Xian-Ming Zhang \u0000 (, )","doi":"10.1007/s40843-024-3081-9","DOIUrl":"10.1007/s40843-024-3081-9","url":null,"abstract":"<div><p>Due to their high capacity, the P2-type layered oxide cathodes containing oxygen redox reaction processes have attracted wide attention for sodium-ion batteries. However, these materials usually exhibit poor electro- chemical properties, resulting from irreversible oxygen redox reactions and phase transition processes at high voltages, and thus hinder their large-scale application. This work reveals the mechanism for the significantly improved cycle stability and rate performance of Co/Ni-free Na<sub>0.75</sub>Li<sub>0.25−2/3<i>x</i></sub>Cu<sub><i>x</i></sub>Mn<sub>0.75−1/3<i>x</i></sub> O<sub>2</sub> <i>via</i> Cu doping. <i>Ex-situ</i> XPS demonstrates that Cu doping reduces the amount of Mn<sup>3+</sup> that triggers the Jahn-Teller effect during the cycling. In addition, the electron enrichment of oxygen around Cu can alleviate the irreversible oxidation of oxygen, and thus suppressing the phase transition originates from the rapid weakening of the electrostatic repulsion between O-O. Meanwhile, <i>in-situ</i> XRD results verify that the Na<sub>0.75</sub>Li<sub>0.19</sub>Cu<sub>0.09</sub>Mn<sub>0.72</sub>O<sub>2</sub> maintains the P2 phase structure during charging and discharging, resulting in a near-zero strain characteristic of 1.9%. Therefore, the optimized cathode delivers a high reversible capacity of 194.9 mAh g<sup>−1</sup> at 0.1 C and excellent capacity retention of 88.6% after 100 cycles at 5 C. The full cell paired with commercial hard carbon anode delivers energy density of 240 Wh kg<sup>−1</sup>. Our research provides an idea for designing a new type of intercalated cathode for sodium-ion batteries with low cost and high energy density.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3629 - 3636"},"PeriodicalIF":6.8,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Cui (, ), Zixuan Jiang (, ), Yu Yang (, ), Siliang Tao (, ), Shuang Wu (, ), Jing Yin (, ), Fei Wang (, ), Guanshi Qin (, ), Fanchao Meng (, ), Dan Zhao (, ), Weiping Qin (, )
{"title":"A strategy for preparing broadband polymer based optical waveguide amplifiers: doping low crystal field symmetric nanocrystals in polymer matrix as gain media","authors":"Hao Cui \u0000 (, ), Zixuan Jiang \u0000 (, ), Yu Yang \u0000 (, ), Siliang Tao \u0000 (, ), Shuang Wu \u0000 (, ), Jing Yin \u0000 (, ), Fei Wang \u0000 (, ), Guanshi Qin \u0000 (, ), Fanchao Meng \u0000 (, ), Dan Zhao \u0000 (, ), Weiping Qin \u0000 (, )","doi":"10.1007/s40843-024-3092-3","DOIUrl":"10.1007/s40843-024-3092-3","url":null,"abstract":"<div><p>Optical waveguide amplifiers are essential devices in integrated optical systems, with their gain bandwidths directly influencing the operating wavelengths of optical circuits. Previous Er<sup>3+</sup>-doped polymer optical waveguide amplifiers have been limited to amplifying signals within the C-band. To achieve broadband polymer optical waveguide amplification, we propose the use of nanocrystals with low crystal field symmetry to extend the working bandwidth. Our approach utilizes LiYF<sub>4</sub>: Yb, Er nanoparticles embedded in poly(methyl methacrylate) as the gain medium, enabling signal amplification from most of the S-band to the whole (C + L) band. The low crystal field symmetry of the LiYF<sub>4</sub> host significantly splits the <sup>4</sup>I<sub>13/2</sub> and <sup>4</sup>I<sub>15/2</sub> levels of Er<sup>3+</sup> ions owing to the crystal field effect, facilitating broadband down-conversion luminescence under 980-nm excitation. Furthermore, a fluorescence kinetic analysis confirms that the broadband luminescence of Er<sup>3+</sup> arises from significant energy-level splitting caused by the crystal field effect. Under 980-nm excitation, the amplifiers exhibited relative gains of approximately 12.6 dB at 1535 nm, 7.4 dB at 1480 nm, and 3.7 dB at 1610 nm. The Er<sup>3+</sup>-doped broadband polymer optical waveguide amplifier was successfully prepared.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 12","pages":"3908 - 3916"},"PeriodicalIF":6.8,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuanjun Zhao (, ), Xinyu Da (, ), Yanyang Qin (, ), Xin Jia (, ), Xuetian Deng (, ), Shujiang Ding (, ), Junqiao Xiong (, ), Qiang Rong (, ), Xiangpeng Kong (, ), Guoxin Gao (, )
{"title":"Nonflammable PVDF-based gel polymer electrolytes modified by dimethyl methylphosphate for wide temperature range, long cycle-life and high-safety lithium metal batteries","authors":"Yuanjun Zhao \u0000 (, ), Xinyu Da \u0000 (, ), Yanyang Qin \u0000 (, ), Xin Jia \u0000 (, ), Xuetian Deng \u0000 (, ), Shujiang Ding \u0000 (, ), Junqiao Xiong \u0000 (, ), Qiang Rong \u0000 (, ), Xiangpeng Kong \u0000 (, ), Guoxin Gao \u0000 (, )","doi":"10.1007/s40843-024-3130-y","DOIUrl":"10.1007/s40843-024-3130-y","url":null,"abstract":"<div><p>Gel polymer electrolytes (GPEs) has been considered as a promising candidate for the development of lithium metal batteries (LMBs) with high energy density and high safety, yet most reported GPEs is flammable, making the LMBs still facing great safety hazards. Herein, we used dimethyl methylphosphate (DMMP) as the functional flame retardant and plasticizer for poly(vinylidene fluoride) (PVDF) matrix to develop a novel nonflammable PVDF-DMMP GPEs for LMBs. The DMMP not only highly enhances the flame resistance of PVDF-DMMP GPEs, the efficient dissociation of lithium salt and the rapid transport of lithium ions, but also helps to form stable and robust CEI/SEI layers. As a result, the ultrathin PVDF-DMMP GPEs (∼20 µm) present superb flame resistance, high ionic conductivity (1.34 × 10<sup>−3</sup> S cm<sup>−1</sup> at 30°C), fast lithium ion transport (<span>(t_{text{Li}^{+}}=0.59)</span> at 30°C), high electrochemical stability voltage window (over 4 V) at 30–80°C and uniform lithium deposition. When used in Li∥Li symmetric cells, Li∥LiFePO<sub>4</sub> (LFP) and Li∥LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> full cells, the nonflammable PVDF-DMMP GPEs could endow these cells with long-term cycle stability, high rate capability, wide-temperature operation ranges (from −20 to 80°C) and high safety simultaneously. Even when suffering from harsh deconstructive tests, the Li∣PVDF-DMMP GPEs∣LFP pouch cells still work normally without any safety hazards. The actual energy density of the packed pouch cell is as high as 508 Wh kg<sup>−1</sup>. Therefore, our work can provide a promising strategy for the design of high safety and high-energy-density LMBs.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 12","pages":"3994 - 4004"},"PeriodicalIF":6.8,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fuchun Nan (, ), Xiaokuang Xue (, ), Jian Li (, ), Ke Liang (, ), Jian Wang (, ), William W. Yu (, ), Jiechao Ge (, ), Pengfei Wang (, )
{"title":"Adenosine triphosphate-responsive carbon dots nanoreactors for T1-weighted magnetic resonance imaging-guided tumor chemodynamic therapy","authors":"Fuchun Nan \u0000 (, ), Xiaokuang Xue \u0000 (, ), Jian Li \u0000 (, ), Ke Liang \u0000 (, ), Jian Wang \u0000 (, ), William W. Yu \u0000 (, ), Jiechao Ge \u0000 (, ), Pengfei Wang \u0000 (, )","doi":"10.1007/s40843-024-3038-8","DOIUrl":"10.1007/s40843-024-3038-8","url":null,"abstract":"<div><p>There are various strategies to conduct tumor microenvironment (TME) stimulus-responsive (e.g., acid, H<sub>2</sub>O<sub>2</sub> or glutathione) nanoreactors for increasing the efficiency of chemodynamic therapy (CDT). Among these, the exploitation of adenosine triphosphate (ATP, another over-expressed biomarker in TME)-responsive nanoreactors for tumor CDT is still challenging. Herein, the ATP-responsive iron-doped CDs (FeCDs) were firstly prepared and then co-assembled with glucose oxidase (GOx) to obtain FeCDs/GOx liposomes as ATP-responsive nanoreactors. Under TME conditions, the nanoreactors initially released FeCDs and GOx. Subsequently, with the existence of ATP, iron ions were rapidly released from the FeCDs to trigger Fenton/Fenton-like reactions for generating ·OH. Meanwhile, the <i>T</i><sub>1</sub>-weighted magnetic resonance imaging (MRI) was achieved due to the released iron ions. Moreover, the GOx converted endogenous glucose in tumor to gluconic acid and H<sub>2</sub>O<sub>2</sub> to satisfy the requirement of ·OH generation. <i>In vitro</i> as well as <i>in vivo</i> experiments illustrated that the obtained ATP-responsive CD nanoreactors could be used as a versatile nanotheranostics for simultaneously <i>T</i><sub>1</sub>-weighted MRI-guided tumor CDT. This work presents a new ATP-responsive nanoreactor with self-supplied H<sub>2</sub>O<sub>2</sub> for multifunctional nanotheranostic applications.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3742 - 3752"},"PeriodicalIF":6.8,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fei Li (, ), Jiongpeng Huang (, ), Dingxin Xu (, ), Chengjin Wang (, ), Liang Zhao (, ), Xinyu Gong (, ), Hang Li (, ), Can Yang Zhang (, ), Qinghua Song (, ), Yang Su (, ), Hui-Ming Cheng (, )
{"title":"A portable and washable solar steam evaporator based on graphene and recycled gold for efficient point-of-use water purification","authors":"Fei Li \u0000 (, ), Jiongpeng Huang \u0000 (, ), Dingxin Xu \u0000 (, ), Chengjin Wang \u0000 (, ), Liang Zhao \u0000 (, ), Xinyu Gong \u0000 (, ), Hang Li \u0000 (, ), Can Yang Zhang \u0000 (, ), Qinghua Song \u0000 (, ), Yang Su \u0000 (, ), Hui-Ming Cheng \u0000 (, )","doi":"10.1007/s40843-024-3089-2","DOIUrl":"10.1007/s40843-024-3089-2","url":null,"abstract":"<div><p>A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage. Previous efforts have made significant advances in maximizing its water evaporation rate, but no single evaporator has all the properties necessary for practical point-of-use application, including a high efficiency for generation of drinkable water, an excellent portability critical for on-site water purification, good washability for mitigating evaporator fouling, and good reusability. We report a strategy to produce a high-performance photothermal material for point-of-use water purification. By simultaneously incorporating graphene and gold particles grown from recycled electronic waste in a mechanically strong sponge, we achieved highly efficient water purification under realistic conditions. In addition to a high evaporation rate (3.55 kg/m<sup>2</sup>/h under one-sun irradiation) attributed to a control of atomic structure of graphene and the size-dependent surface plasmon resonance of gold nanoparticles, it is portable which can be folded, vacuum compacted, dried and rehydrated without compromising performance. It also allows repeated washing to remove contaminant fouling so that it can be reused. The evaporator transforms various types of contaminated water into drinkable clean water, and can be mounted at any angle to optimize the incident solar irradiation. Furthermore, the assembled steam evaporator device could gain purified water meeting the World Health Organization drinking water standards with a high evaporation rate of 9.36 kg/m<sup>2</sup>/h under outdoor sunlight.</p></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3700 - 3709"},"PeriodicalIF":6.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li Shi (, ), Hanbo Wu (, ), Wendi Xu (, ), Wei Fu (, ), Xiaobing Wang (, ), Zhengyu Gu (, ), Xiuyun Zhang (, ), Jianyu Chen (, ), Yanwen Ma (, ), Jin Zhao (, )
{"title":"Electrocatalytic conversion of CO2 to CH4 over Cu-based cluster via atomically precise local environment modulation","authors":"Li Shi \u0000 (, ), Hanbo Wu \u0000 (, ), Wendi Xu \u0000 (, ), Wei Fu \u0000 (, ), Xiaobing Wang \u0000 (, ), Zhengyu Gu \u0000 (, ), Xiuyun Zhang \u0000 (, ), Jianyu Chen \u0000 (, ), Yanwen Ma \u0000 (, ), Jin Zhao \u0000 (, )","doi":"10.1007/s40843-024-3088-5","DOIUrl":"10.1007/s40843-024-3088-5","url":null,"abstract":"<div><p>The development of low-cost, high-performance catalysts at the atomic scale has become a challenging issue for the large-scale applications of renewable clean energy technologies. Herein, on the basis of density functional theory calculation, we systematically investigate the effect of the local environment on the activity and selectivity of electrochemical carbon dioxide reduction reaction over single/multi-atom alloy clusters formed by the transition metal (Fe, Co, and Ni)-doped Cu13/55 clusters. Our findings reveal that the catalytic performance of multi-atom alloy clusters far exceeds that of Cu (211) surface. Notably, the Co666 configuration exhibits exceptional performance with a remarkably low free energy barrier of just 0.33 eV. Furthermore, our investigations demonstrate that catalytic performance is predominantly determined by the relative proportion of modifying metallic dopant species that generate a coordination number of 6. This ratio principally influences the adsorption strength of key intermediates (HCOO* and H<sub>2</sub>COO*). Bader charge analyses and free energy calculations elucidate a new mechanistic pathway, wherein the hydrogenation of CO<sub>2</sub> at C-sites catalyzes the reduction of CO<sub>2</sub> to CH<sub>4</sub>. This theoretical research provides valuable insights into the fundamental processes and energy landscapes involved in converting CO<sub>2</sub> to CH<sub>4</sub> on the studied catalytic structure, potentially paving the way for more efficient and sustainable carbon dioxide utilization strategies.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3602 - 3608"},"PeriodicalIF":6.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540689","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaoyi Lai (, ), Junqing Wang (, ), Xiaolong Liu (, ), Lei Hua (, ), Bin Li (, ), Weiguo Zhu (, ), Jun Yeob Lee, Yafei Wang (, )
{"title":"Effective exciplex system with high emission efficiency via intramolecular hydrogen bonding for efficient solution processable OLEDs","authors":"Xiaoyi Lai \u0000 (, ), Junqing Wang \u0000 (, ), Xiaolong Liu \u0000 (, ), Lei Hua \u0000 (, ), Bin Li \u0000 (, ), Weiguo Zhu \u0000 (, ), Jun Yeob Lee, Yafei Wang \u0000 (, )","doi":"10.1007/s40843-024-3067-x","DOIUrl":"10.1007/s40843-024-3067-x","url":null,"abstract":"<div><p>Exciplex system is a charming candidate for thermally activated delayed fluorescence (TADF) due to its intrinsic small energy difference between the lowest singlet state and triplet excited state (Δ<i>E</i><sub>ST</sub>). However, high emission efficiency and fast radiative decay rate are still a formidable task for the exciplex emission. Herein two novel tri(triazolo) triazine-based TADF emitters, named TTT-HPh-Ac and TTT-MePh-Ac, are synthesized and characterized. Using such TADF emitters as the donor molecule and (1,3,5-triazine-2,4,6-triyl)tris(benzene-3,1-dial)tris(diphenylphosphine oxide) (PO-T2T) as the acceptor molecule, the exciplex system of TTT-HPh-Ac:PO-T2T and TTT-MePh-Ac:PO-T2T are prepared, which show a tiny Δ<i>E</i><sub>ST</sub> of 40 ± 20 meV and fast reverse intersystem crossing rate. As a result, very high emission efficiency (97%) and a small non-radiative decay rate are detected for the exciplex TADF system. The solution processable organic light-emitting diode using the exciplex system as the emitter achieves a maximum external quantum efficiency (EQE<sub>max</sub>) of 17.0%. When using the exciplex as the host matrix, the TTT-MePh-Ac:PO-T2T based solution processable device shows a better performance with an EQE<sub>max</sub> of 20% with a very small efficiency roll-off of 6% at 1000 cd m<sup>−2</sup>. This work proves that the molecule with both intramolecular hydrogen bonding and proper twisted molecular geometry in exciplex is more favorable to enhance its emission efficiency and suppress the non-radiative transition, which provides a new way to develop efficient and stable exciplex emitters.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3543 - 3552"},"PeriodicalIF":6.8,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号
