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Science Advances · 2022 ·Vol. 8 ·期 30 · IF 14.957

Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

Min Lu,Yao Zheng,Yang Hu,Bolong Huang,Deguang Ji,Mingzi Sun,Jianyi Li,Yong Peng,Rui Si,Pinxian Xi,Chun-Hua Yan

The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various LaxSr1−xCoO3−δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on LaxSr1−xCoO3−δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts.

CAS / MDL: 64-17-5 67-63-0
研究领域: 电化学 · 催化科学
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Journal of Materials Chemistry A · 2025 · IF 9.5

Demonstration of 650°C operating high-performance metal-supported solid oxide fuel cell using Gd-doped CeO2 electrolyte, Ni anode and Sm(Ba0.5Sr0.5)Co2-xFexO5+δ- Ce0.9Gd0.1O2-δ cathode

Fei-Fei Lu,Jia-Hong Li,Qi Ma,Changjiu Li,Venkataraman Thangadurai,Chengxin Li

Metal-supported solid oxide fuel cells (MS-SOFCs) exhibit numerous advantages, including thermal cycle stability, rapid start-up and lower costs. However, the slow oxygen reduction reaction (ORR) at the cathode, especially at intermediate-low temperatures, poses a critical challenge to the development of MS-SOFCs. Here, we report a synergistic effect of co-doping in a cation-ordered double perovskite type material, Sm(Ba0.5Sr0.5)Co2-xFexO5+δ (SBSCFx), which has enhanced catalytic activity for ORR and chemical compatibility with Ce0.9Gd0.1O2-δ (GDC). X-ray photoelectron spectroscopy and thermogravimetric analysis were used to examine how Fe-doping in SBSCFx impacts the functional properties. A composite cathode with GDC was further prepared to enhance thermal compatibility with GDC, which effectively reduces the thermal expansion of the SBSCFx cathode from 23.35×10-6 K-1 to 15.04×10-6 K-1. The electrochemical results of symmetrical cells and the DRT fitting analysis demonstrate that the SBSCFx-GDC composite cathode exhibits strong ORR activity. Notably, the SBSCF10-GDC composite cathode achieves a remarkably low polarization resistance of 0.05 Ω·cm² at 650°C. The metal-supported single cell with SBSCF10-GDC cathode exhibited an open-circuit voltage of 0.85 V and showed a peak power density of 833 mW cm-² at 650℃. Furthermore, its stability during long-term cell operation highlights its potential as a cathode for intermediate-low temperature metal-supported SOFCs.

研究领域: 能源材料科学 · 电化学工程
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Stable cyan and white light-emitting diodes enabled by branched cations sterically stabilized 2D/3D perovskites

Yueyue Shen,Huilin Tang,Feng Liu,Kebin Lin,Jianxun Lu,Chuanzhong Yan,Wenjing Feng,Kaikai Liu,Liqin Wu,Mingjie Li,Zhanhua Wei,Keyou Yan

As an indispensable part of the visible light region, cyan emission (470 nm–500 nm) is of great importance in lighting, displays, and light communication. Metal halide perovskite materials have made significant progress in the field of luminescent materials and devices. However, the corresponding cyan emission through halide mixing is non-stable due to halogen migration and phase separation. Herein, we developed a steric stabilization approach to tune and stabilize the cyan emission of methylammonium (MA)-based perovskites. Dimethylammonium (DMA + ) lead bromide, with the small DMA + branched cation, was used as intermediate to react with MABr, forming blue-to-green emissive (MA) x (DMA)PbBr 3 +x compounds simular to the low-dimensional perovskites. Furthermore, protonated (trimethylsilyl)methylamine (TmMA), the larger branched cation, was adopted as an interlayer space to further reduce the perovskite dimension, tuning the emission to the cyan region. The combination of the two branched cations enabled us to achieve a champion photoluminescence quantum yield (PLQY) of ~87.8% (peak wavelength ~486 nm). Moreover, the as-synthesized double cations modified perovskites in combination with  LED InGaN chip can be used to fabricate stable cyan emission LEDs with improved durability (over 1000 min) and white LEDs with increased color rendering index (from ~73.1 to ~81.7).

研究领域: 材料科学 · 光学工程
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RSC Advances · 2020 ·Vol. 10 ·期 59 ·35740-35752 · IF 3.119

Solar thermochemical CO2 splitting with doped perovskite LaCo0.7Zr0.3O3: thermodynamic performance and solar-to-fuel efficiency

Lei Wang,Tianzeng Ma,Shaomeng Dai,Ting Ren,Zheshao Chang,Mingkai Fu,Xin Li,Yong Li

The research of thermochemical CO2 splitting based on perovskites is a promising approach to green energy development. Performance evaluation was performed towards the doped perovskite LaCo0.7Zr0.3O3 (LCZ-73) based two-step thermochemical CO2 splitting process thermodynamically based on the experimentally derived parameters for the first time. The impacts of vacuum pump and inert gas purge to reduce oxygen partial pressure and CO2 heating on the performance parameter ηsolar-to-fuel have been analyzed. The results showed that at the PO2 of 10−5 bar, non-stoichiometric oxygen δ increased by more than 3 times as the reduction temperature varied from 1000 °C to 1300 °C, however, no significant deviation of δ was observed between 1300 °C and 1400 °C. The reaction enthalpy ranged from 60 to 130 kJ mol−1 corresponding to δ = 0.05–0.40. Comparing the abovementioned two ways to reduce the oxygen partial pressure, the ηsolar-to-fuel of 0.39% and 0.1% can be achieved with 75% and without heat recovery with the CO2 flow rate of 40 sccm under experimental conditions, respectively. The energy cost for CO2 heating during the thermodynamic process as the nCO2/nLCZ-73 increases was obtained from the perspective of energy analysis. The ratio of nCO2/nLCZ-73 at lower temperature required more demanding conditions for the aim of commercialization. Finally, the ability of perovskite to split CO2 and thermochemical performance were tested under different CO2 flow rates. The results showed that high CO2 flow rate was conducive to the production of CO, but at the cost of low ηsolar-to-fuel. The maximum solar-to-fuel efficiency of 1.36% was achieved experimentally at a CO2 flow rate of 10 sccm in the oxidation step and 75% heat recovery.

研究领域: 能源科学 · 材料科学 · 化学工程
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RSC Advances · 2021 ·Vol. 11 ·期 11 ·5874-5884 · IF 3.361

Mechanochemical synthesis of pure phase mixed-cation/anion (FAPbI3)x(MAPbBr3)1−x hybrid perovskite materials: compositional engineering and photovoltaic performance

Sheng Tang,Xinyu Xiao,Jing Hu,Bo Gao,Hunglin Chen,Zhuang Zuo,Qi Qi,Zongyang Peng,Jianchun Wen,Dechun Zou

Organic–inorganic hybrid perovskites have emerged as promising light harvesting materials for many optoelectronic devices. Here, we present a facile mechanochemical synthesis (MCS) route for the preparation of a series of pure phase mixed-cation/anion (FAPbI3)x(MAPbBr3)1−x (0 ≤ x ≤ 1) hybrid perovskite materials for high-efficiency thin-film perovskite solar cells (PSCs). The use of (α-FAPbI3)0.95(MAPbBr3)0.05 perovskite prepared by MCS for the thin-film PSCs achieves a maximum PCE of 15.9% from a current–voltage (J–V) scan, which stabilises at 15.4% after 120 s of the maximum power point output. Furthermore, PSCs based on (KPbI3)0.05(FAPbI3)0.9(MAPbBr3)0.05 perovskite prepared by MCS exhibit higher photovoltaic performance and lower hysteresis compared with (α-FAPbI3)0.95(MAPbBr3)0.05, with a maximum PCE of 16.7%. These results indicate that the use of mechanochemically synthesised perovskites provides a promising strategy for high performance PSCs and superior control in optoelectronic properties, leading to improved control in fabrication approaches and facilitating the development of efficient and stable PSCs in the future.

研究领域: 材料科学 · 能源科学 · 光电子学
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PHYSICA B-CONDENSED MATTER · 2022 · IF 2.988

Green anti-solvent processed white light emitting perovskite phosphors in one step

Bing Wang,Yingdu Liu,Zhiliang Deng,Pei Li,Wanfu Wang,Xiaoping Ouyang,Qiang Xu

Despite the excellent properties of perovskite materials, the strict oxygen-free atmosphere, heating temperature and a large number of toxic solvents applied during preparation obstruct their more widespread applications. Using ethanol as a green anti-solvent to successfully prepare a series of copper-based perovskite micro-phosphors. They have a luminescence peak between 445 nm and 580 nm adjusted with halogen and the highest PLQY of 81.6%. Moreover, by simply adjusting the molar ratio of CsI to CuI, white-light emission phosphors can be synthesized in one step. It exhibits a Commission Internationale de L'Eclairage (CIE) chromaticity coordinates (0.35, 0.35) and a correlated color temperature (CCT) of 4798 K. After two months of storage, there is still 97.4% of the initial light intensity . This technology offers a green and straightforward method for producing perovskite phosphors.

研究领域: 材料科学 · 光学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

A promising Nb-doped La0.5Sr0.5Co0.8Cu0.2O3–δ cathode materials for intermediate temperature solid oxide fuel cells

Ru-Yi Chen,De-Feng Zhou,Xiao-Fei Zhu,Ning Wang,Jing-He Bai,Chun-Qi Guo,Lian Ai

Cobalt-based perovskites are widely used as cathode materials for intermediate temperature solid oxide fuel cells (IT-SOFCs) due to their excellent catalytic activities. In this paper, a series of Nb-doped La 0.5 Sr 0.5 Co 0.8 Cu 0.2- x Nb x O 3–δ (LSCCu 0.2- x Nb x O 3-δ , x  = 0.00 ≤  x  ≤ 0.075) cathode materials with excellent electrochemical performance are prepared by a Pechini method, and the critical Nb-doping effect is studied in detail. In the new cathode material, the surface oxygen content increases with the Nb doping, while the segregation of Sr and the coefficient of thermal expansion (TEC) is reduced. The optimum LSCCu 0.15 Nb 0.05 O 3-δ shows the highest surface oxygen content, the lowest surface Sr content, and the highest oxygen reduced reaction (ORR) catalytic activity. At 700 °C, the polarization resistance (Rp) is 0.065 Ω cm 2 , and the peak power density (PPD) of single cells supported by the electrolyte is 518 mW cm −2 , which are promising for the IT-SOFCs. Therefore, the LSCCu 0.15 Nb 0.05 O 3-δ should be a promising cathode material for the high-performance IT-SOFCs.

研究领域: 材料科学 · 能源科学
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JOURNAL OF HAZARDOUS MATERIALS · 2018 · IF 6.434

Heterogeneous activation of peroxymonosulfate by LaCo1-xCuxO3 perovskites for degradation of organic pollutants

Sen Lu,Guanlong Wang,Shuo Chen,Hongtao Yu,Fei Ye,Xie Quan

Recently cobalt-based heterogeneous catalysts have been widely investigated for peroxymonosulfate (PMS) activation in sulfate radical-based advanced oxidation processes. However, the improvement of the catalytic performance for PMS activation remains to be a challenge. As the limiting step, the rapid transformation of Co II /Co III redox pairs is crucial for PMS activation. Perovskites attract increasing attention due to their controllable oxidation state of B-site metal and formation of oxygen vacancies, which accelerates the cycle of redox pairs. LaCo 1-x M x O 3 (M = Cu, Fe and Mn) perovskites as heterogeneous catalysts of PMS were synthesized for the degradation of phenol. The results showed that LaCo 0.4 Cu 0.6 O 3 exhibited the highest catalytic activity. The pseudo first-order kinetic constant of phenol degradation on LaCo 0.4 Cu 0.6 O 3 is 0.302 min −1 , being about 5 times as high as Co 2+ with same molar concentration of cobalt in LaCo 0.4 Cu 0.6 O 3 . XPS analysis confirmed that substitution of copper could promote the cycle of Co II /Co III , thus enhance the catalytic efficiency for PMS activation. The facilitated cycle of Co II /Co III played a crucial role in the generation of sulfate radicals, hydroxyl radicals and singlet oxygen. And sulfate radical was the primary radical responsible for pollutants degradation. The results provide insights into constructing novel perovskite catalysts for the removal of organic pollutants in water.

研究领域: 环境科学 · 化学工程
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Journal of Materials Chemistry B · 2018 ·Vol. 6 ·期 37 ·5931-5939 · IF 4.776

Oxidase-mimicking activity of perovskite LaMnO3+δ nanofibers and their application for colorimetric sensing

Lifei Song,Yun Zhu,Zezhou Yang,Ce Wang,Xiaofeng Lu

Nanomaterials with ABX3-type perovskite structure have attracted considerable and increasing attention due to their unique physical and chemical properties as well as promising applications in various fields. In this work, we have developed a simple electrospinning followed by a calcination process to prepare ABO3-type perovskite LaMnO3+δ nanofibers as efficient oxidase mimics for the detection of L-cysteine. The oxidase-like catalytic activity of the prepared LaMnO3+δ nanofibers is heavily dependent on the calcination temperature which results in different sizes of the LaMnO3+δ crystals and their crystallinity, and the maximum activity is achieved at the calcination temperature of 700 °C. Based on the high oxidase-like catalytic activity of the as-prepared perovskite LaMnO3+δ nanofibers, a simple and accurate colorimetric detection method towards L-cysteine has been developed. The detection limit is as low as 109.8 nM and an excellent selectivity for L-cysteine detection with common substances in human blood as interferents is also achieved. In addition, the LaMnO3+δ nanofibers can be retained as a monolithic membrane after the calcination process, making them an oxidase mimic for on-demand colorimetric sensing. This work reveals the promising prospects for the perovskite LaMnO3+δ materials in biosensing, medical diagnosis, food safety and environmental monitoring.

CAS / MDL: 67-68-5
研究领域: 生物传感 · 医学诊断 · 食品安全 · 环境监测
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CERAMICS INTERNATIONAL · 2015 · IF 2.605

A novel cobalt-free double-perovskite NdBaFe1.9Nb0.1O5+δ cathode material for proton-conducting IT-SOFC

Xinbo Mao,Wenbao Wang,Guilin Ma

A novel cobalt-free double-perovskite oxide NdBaFe 1.9 Nb 0.1 O 5+ δ (NBFNb10) was prepared by a solid-state reaction method and investigated as a suitable cathode material for intermediate temperature solid oxide fuel cells (IT-SOFCs). It was discovered that partial substitution of Nb for Fe-site further enhanced the electrical conductivity of NdBaFe 2 O 5+ δ (NBF). The NBFNb10 exhibited the highest conductivity of 109   S   cm −1 at 300–800   °C in air, and showed good chemical compatibility with the BaZr 0.1 Ce 0.7 Y 0.2 O 3− α (BZCY) electrolyte. A single cell with the NBFNb10–BZCY composite cathode and NiO–BZCY composite anode-supported BZCY electrolyte membrane (ca. 30   μm thickness) was fabricated and tested at 500–700   °C using H 2 as fuel and air as oxidant. The peak power density and the interfacial polarization resistance ( R p ) were 392   mW   cm −2 and 0.14   Ω   cm 2 at 700   °C, respectively.

CAS / MDL: 1314-23-4 1313-96-8
研究领域: 材料科学 · 能源科学
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Materials Advances · 2023 ·Vol. 4 ·期 10 ·2365-2371 · IF 5

Sn2+ doping-induced large extra vibrational energy of an excited state for efficient blue emission in Cs2SnCl6:Bi

Shaofan Fang,Jinbo Huang,Huixia Li,Jingheng Nie,Zexiang Liu,Feier Fang,Haizhe Zhong

Luminescent metal halides doped with ns2-metal ions, such as 6s2-metal Bi3+, show excellent optoelectronic properties. However, the origin of the high photoluminescence quantum yield (PLQY) of Cs2SnCl6:Bi remains controversial and unclear. In this study, a series of Cs2SnCl6:Bi were synthesized by adopting different tin precursors of SnCl2/SnCl4. The samples from SnCl2 exhibited much higher PLQY than those from SnCl4, and the doping concentrations of Bi3+ had little effect on the high PLQY. When H3PO2 is added to the precursor of SnCl4 to reduce Sn4+ to Sn2+, the prepared Cs2SnCl6:Bi shows bright emission light and high PLQY. The high PLQY of Cs2SnCl6:Bi is attributed to the co-doping of Bi3+ and Sn2+. [SnCl4]2− and two VCl induce a large extra vibrational energy of the heavy localized excitons from [BiCl5]2− to enhance the efficiency of radiative recombination for high PLQY. This work deepens the understanding of the luminescence mechanism of Cs2SnCl6:Bi and supplies significant references for developing more perovskite materials with outstanding luminescence.

CAS / MDL: 6303-21-5 10025-69-1
研究领域: 材料科学 · 光电 · 化学
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Materials Horizons · 2025 · IF 10.7

Suppressing thermal degradation of CsPbBr3 quantum dot/EVA films via APTES-mediated interface engineering: toward efficient and stable luminescence down-shifting for silicon solar cells

Hongfei Liang,Lu Chen,Yang Wu,Youwen Xue,Yuxuan Wang,Wenjie Ji,Huanqi Cao,Qian Zhao,Jian Song,Guoran Li

Luminescence down-shifting technology is increasingly recognized as a crucial option for enhancing the efficiency of silicon solar cells. However, high-quality down-shifting materials, such as perovskite quantum dots, face challenges related to poor thermal stability. These materials tend to agglomerate into larger sizes, leading to the deterioration of the luminescence films at high temperature. Unlike introducing a protecting layer on perovskite quantum dots, we applied 3-aminopropyltriethoxysilane (APTES) as a direct capping agent for perovskite quantum dots in this work to achieve both efficient and stable composite down-shifting films. The interaction between APTES and CsPbBr3 quantum dots is thoroughly analyzed using both experimental measurements and theoretical calculations. Due to the strong interaction between APTES and CsPbBr3, an optimal amount of APTES effectively stabilizes the quantum dots. When mixed with ethylene-vinyl acetate (EVA) copolymer, the strong interaction between APTES and polymer chains could suppress the aggregation of CsPbBr3 quantum dots and inhibit degradation of the composite film under heating. Upon coating on commercial crystalline silicon solar cells, the optimal CsPbBr3 quantum dot/EVA composite film achieves an absolute efficiency by 1.00%, maintaining a 0.81% efficiency improvement even after annealing at 90 °C for 3 hours. In contrast, while the film without APTES shows an efficiency improvement of 0.63% at room temperature but experiences a decrease of 0.23% under the same heating conditions. This work provides a feasible strategy to enhance the thermal stability of CsPbBr3 quantum dot/EVA composite films under high-temperature conditions, offering a promising path toward the commercial application of perovskite-based luminescence down-shifting films in silicon solar cells.

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