DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 8
·2392-2403
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IF 4
Amir Said,Guanyun Zhang,Caiyun Liu,Dexin Wang,Huihui Niu,Yanshu Liu,Guanjie Chen,Chen-Ho Tung,Yifeng Wang
The cycloaddition reaction of CO2 to epoxides is quite promising for CO2 capture and storage as well as the production of value-added fine chemicals. Herein, a novel atomically precise lead-doped titanium-oxide cluster with the formula Ti10Pb2O16(phen)4(Ac)12(DMF)2 (denoted as Ti10Pb2; phen = 1,10-phenanthroline; Ac = acetate; DMF = dimethylformamide) was synthesized through a facile solvothermal process, and is a molecular photocatalyst with surface-anchored main-group metal active sites. Its structure was characterized by single-crystal X-ray diffraction and other complementary techniques. Ti10Pb2 showed high photo-response and charge-separation efficiency under simulated sunlight irradiation. Ti10Pb2 was successfully used in the cycloaddition reaction of CO2 with epoxides under solvent-free conditions. While its catalytic activity due to the Lewis acidity was moderate, simulated solar light irradiation further enhanced the reaction rate, demonstrating the synergistic effect of photocatalysis and Lewis-acid thermocatalysis.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Xiaojing Dong,Jintao Wang,Yue Hao,Yiqiang Sun,Xu Zhang,Bo Xu,Cuncheng Li
Exploring oxygen evolution reaction (OER) electrocatalysts over a universal pH range to simultaneously achieve enhanced activity, improved stability and reduced cost is a rewarding yet challenging endeavor. Considering the hydrophilicity and electronegativity disparity between Pb and Ru, herein, a Pb doped RuO 2 catalyst and its application as electrocatalyst for OER under universal pH conditions are studied. Due to the modified hydrophilicity and electronic structure, the Pb 0.1 Ru 0.9 O 2 only requires an overpotential of 207 mV to obtain a current density of 10 mA cm −2 in acidic environment, and overpotentials of 232 mV and 363 mV are required in alkaline and neutral environments, respectively. Moreover, extensive stability assessments conducted over a 24-h period reveal remarkable stability of the catalyst in diverse environments, encompassing acidic, alkaline, and neutral conditions. Additionally, the utilization of density functional theory (DFT) computations offers persuasive evidence that the inclusion of Pb within RuO 2 can significantly alter its electronic configuration, thereby promoting efficient electron transfer processes. This modulation of the electronic structure is crucial for enhancing the catalytic performance of the material. This research paves the way for innovative designs of highly efficient oxygen evolution reaction (OER) catalysts, featuring minimized use of precious metals, heightened catalytic prowess, and unparalleled stability across a broad pH range.
研究领域:
材料科学
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电化学
·
催化
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DOI
高影响因子
CRYSTENGCOMM
·
2015
·Vol. 17
·期 45
·8697-8702
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IF 4.034
Xiaolin Wu,Jiang-Long Wang,Hongrui Zhang,Shufang Wang,Shengjun Zhai,Yaguang Li,Dogheche Elhadj,Guangsheng Fu
c-axis oriented Bi1−xPbxCuSeO (0 ≤ x ≤ 0.8) single crystalline thin films have been successfully epitaxially grown on SrTiO3 (001) substrates via the pulsed laser deposition technique. Detailed X-ray diffraction and transmission electron microscopy measurements reveal the excellent c-axis and ab-plane texture of the films. As the Pb doping concentration increases, both the resistivity and the Seebeck coefficient decrease due to the increase in hole carrier concentration. The highest power factor of about 1.2 mW m−1 K−2 has been achieved in Bi0.96Pb0.06CuSeO single crystalline thin films at 673 K, which is much higher than those of polycrystalline ceramics with random orientation, suggesting that c-axis oriented BiCuSeO-based single crystalline thin films might have great potential for application in thermoelectric thin film devices.
研究领域:
材料科学
·
物理学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 30
·6894-6898
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IF 4.857
Shuyu Zhou,Congping Li,Hao Fu,Jing Cao,Jian Zhang,Lei Zhang
Graphical Outstanding resemblance ! The first molecular model of perovskite PbTiO 3 has been successfully prepared by bottom-up assembly of lead-doped titanium-oxo clusters in the presence of p - tert -butylthiacalix[4]arene as stabilizing ligands. Structural characterization confirmed that the clusters have almost the same structure as that in PbTiO 3 (see figure). The nanoclusters showed high solution stability and can be applied as electron-transport materials in perovskite solar cells to give satisfactory efficiencies and high device stability. In this work we have successfully prepared two lead-doped titanium-oxo clusters with core structures that resemble isolated perovskite PbTiO 3 species. In the obtained highly symmetric Pb 8 Ti 7 -oxo cluster, the central TiO 6 octahedra are orthogonally extended to adjacent octahedra through corner-sharing and the eight dopant lead ions form a cubic arrangement, making it the first molecular model of perovskite PbTiO 3 . Moreover, the clusters readily dissolved in chloroform and showed high solution stability, as confirmed by MALDI-TOF MS measurements. Based on such solution processability, they can be easily spin-coated to form homogeneous films, which were employed as electron-transport materials in perovskite solar cells to give an average power conversion efficiency of around 15 % and improved device stability. This newly developed bottom-up cluster assembly method provides an efficient approach to the construction of atomically precise models of perovskite metal oxides as well as potential molecular tools to extend their applications.
研究领域:
材料化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 8
·3666-3674
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IF 3.5
Amir Said,Guanjie Chen,Guanyun Zhang,Dexin Wang,Yanshu Liu,Fangfang Gao,Guo Wang,Chen-Ho Tung,Yifeng Wang
Titanium-oxide clusters (TOCs) are well-defined molecular models for TiO2 materials and provide the opportunity to study the structure–activity relationships of TiO2. Here, we report a new Pb-doped TOC, Ti12Pb2, which resembles a two-layer decker of the {TiTi6} structural units of rutile TiO2 with two Ti4+ ions replaced by two Pb2+ ions. Its electronic structure, photoresponse, and photocatalytic performances were investigated and compared with those of the Ti14 cluster, which is isostructural to Ti12Pb2. Our results indicate that Pb2+ does not affect the electronic structure, but it greatly enhances the photocatalytic activity by improving the charge-separation and interfacial charge-transfer properties of the TOC. The successful synthesis of Ti12Pb2 highlights the roles of closed-shell heterometal ions in the construction of new TOCs. Our mechanism may be an inspiration for understanding the structure–activity relationships of closed-shell heterometal-doped TiO2.
研究领域:
材料科学
·
化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Tingyan Huang,Yu Zhang,Jia Sun,Yinsheng Gu,Fang Wang,Ying-Wei Lu,Paifeng Luo
In recent years, there has been some interest in the use of chemical vapor deposition (CVD) for the fabrication of perovskite solar cells (PSCs) due to its satisfactory film-quality, high controllability and consistency, low equipment cost, and easy industrial scale-up. In this paper, the mixed-cation MAxFA1–xPbI3–yBry perovskite light absorbing films were first deposited via a lead bromide (PbBr2) precursor doped CVD process, and the effect of bromine content on its material phase composition, film morphology, optical band gap, device photovoltaic characteristic, charge recombination, and carrier transport property were systematically studied. The experimental results show that introducing an appropriate PbBr2 doping amount can inhibit the formation of undesirable nonphotoactive γ phase, which enhances the crystallization ability, increases the grain size and material band gap of perovskite films, and then suppresses the carrier recombination, reduces the contact resistance, and facilitates the carrier extraction and transport at the interface. This ultimately leads to an improvement in the power conversion efficiency (PCE) and stability of the PSCs. Consequently, the optimized MAxFA1–xPbI3–yBry PSCs with 0.05 M PbBr2 doping achieve an impressive PCE of 17.94%, which is significantly higher than that of the undoped devices (16.69%) and reaches the high level of PSCs with a hybrid chemical vapor deposition (HCVD) method.
研究领域:
材料科学
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太阳能电池技术
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化学工程
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产品关联
DOI
高影响因子
RARE METALS
·
2025
·Vol. 44
·期 5
·3339-3350
·
IF 11
Wang Wen-Ying,Zhu Jun-Liang,Bo Lin,Zhou Wen-Ying,Liu Xing-Shuo,Li Chang-Cun,Zhang Zheng,Zhao De-Gang
The rock-salt cubic SnSe compound with multiple valleys and inherent low thermal conductivity is considered to be a promising thermoelectric compound. In this study, heterogeneous Pb atoms were strategically introduced into the lattice of cubic SnSe matrix, synergistically adjusting the thermoelectric transport properties of samples by optimizing hole carrier concentration ( n ) and suppressing thermal conductivity ( κ tot ). When the doping content reached 0.08 mol, the peak power factor (PF) at 300 K increased to 20.00 μW·cm –1 ·K –2 . The growing internal microstrain induced by the differences in atomic size strengthened the phonon scattering and effectively reduced the lattice thermal conductivity ( κ L ). With further decoupling of the electrical and thermal transport properties, a peak thermoelectric figure of merit ( ZT ) of 0.82 and an average ZT of 0.42 (300–750 K) were achieved in the samples doped with 0.10 mol Pb. These findings highlight the effectiveness of the selected dopants and demonstrate their synergy in improving the performance of thermoelectric materials. Graphical
研究领域:
材料科学
·
凝聚态物理
·
能源材料
·
热电转换
·
半导体物理
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产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 85
·69878-69885
·
IF 3.84
Guang-Kun Ren,Jin-le Lan,Sajid Butt,Kyle J. Ventura,Yuan-Hua Lin,Ce-Wen Nan
BiCuSeO oxyselenides have been successfully fabricated by self-propagating high-temperature synthesis (SHS). Compared with the SHS process of binary or ternary alloys, thermal analysis indicates the ignition temperature of quaternary layered BiCuSeO oxyselenides approaches the second lower melting point of the compound. The ZT value of SHS-synthesized BiCuSeO is almost 1.5 times larger than that of the solid state reaction (SSR) product at 873 K. This is attributed to the existing amorphous region, nano-pores, and optimized grain size. Furthermore, with the partial substitution of Pb2+ for Bi3+, ZT was enhanced through the optimization of charge carrier concentration and band gap narrowing. This achieved a ZT of 0.91 at 873 K for Bi1−xPbxCuSeO (x = 0.04). Combining with the Debye–Callaway model analysis, the ultralow lattice thermal conductivity of BiCuSeO can potentially be derived from the synergistic effect of intrinsic point defects, efficient grain boundaries and some other mechanisms.
研究领域:
材料科学
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凝聚态物理
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无机非金属材料
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能源材料
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热电转换
✓ 已验证
DOI
高影响因子
Aggregate
·
2025
·Vol. 6
·期 9
·e70112
·
IF 13.7
Zhi-Wei Chen,Na Lin,Xin-Yue Zhang,Yu-Sha Yan,Li Xiao,Yi-Fan Wu,Cheng-Yang Yue,Dongpeng Yan,Xiao-Wu Lei
Underwater blue-emitting X-ray scintillator is important for the resource exploration and communication in deep sea, but remains a significant challenge for perovskites. Herein, we proposed a universal Pb 2+ -doping strategy toward a family of stable 0D Zn halide A n ZnBr 4 realizing highly efficient blue-emitting scintillation. First-principles calculations indicate that doped-Pb 2+ introduced extremely narrow impurity bands, which prompt more carriers into conduction bands, leading to near-unity PLQY. Meanwhile, these halides can withstand complex aqueous solutions containing various chemical substances in wide pH range (1–14) demonstrating ultrahigh water-resistance stabilities. More significantly, these halides exhibit satisfactory scintillation and imaging performance with highest light yield (31,500 photons MeV −1 ), low detection limit (141.2 n Gy air s −1 ) and large spatial resolution (15.10 lp/mm), ranking among the top-performing Zn halide scintillators reported to date. The high water-resistance stabilities and satisfactory scintillation performance endow these halides advanced underwater X-ray imaging. This work not only provides a universal strategy to explore highly-efficient blue-emitting perovskite scintillators, but also realizes application of high-resolution X-ray imaging in underwater environment.
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DOI
高影响因子
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