FUEL
·
2024
·
IF 6.7
Caijun Deng,Chaofan Qi,Zongping Xue,Kai Cui,Xiaomin Wu,Guohua Jing,Huawang Zhao
Hydrogen is a promising clean energy source, and formic acid serves as a significant hydrogen storage material. The electrocatalytic reduction of carbon dioxide (ECO 2 RR) is a promising approach to produce fromate. However, the challenge lies in developing high-performance electrocatalysts for the conversion of CO 2 to formate, due to the limited intrinsic activity, conductivity, and the low density of active sites. In this work, we have fabricated highly active and selective CH 3 COO(BiO) (BiOAc) nanosheets. These nanosheets undergo a transformation into Bi clusters-BiO 2 CO 3 during electrolysis, endowing the material with superior electrocatalytic capabilities for CO 2 reduction to formate, with a Faradaic selectivity of over 90 % across a wide potential window from −0.8 to −1.3 V. Additionally, this catalyst can sustain high current densities above 80 mA cm −2 at low applied potentials without compromising selectivity in a H type electron reactor. Both density functional theory (DFT) and in situ attenuated total reflection-infrared spectroscopy (in situ ATR-IR) findings indicate that the Bi 3+ with reduced density facilitate the activation of CO 2 to *CO 2 , while the charge density-enriched Bi 0 atoms in Bi cluster promote the capture of HCO 3 – and enhance subsequent proton-coupled electron transfer reactions. Collectively, these factors significantly reduce the energy barrier for *OCHO formation on BiOAc, thereby enhancing its catalytic activity and Faradaic efficiency for the electroreduction of CO 2 .
研究领域:
材料科学
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环境科学
·
电化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 26
·2214660
·
IF 19
Zeng-Kui Zhu,Tingting Zhu,Jianbo Wu,Shihai You,Panpan Yu,Xitao Liu,Lina Li,Chengmin Ji,Junhua Luo
2D chiral hybrid perovskites have recently emerged as outstanding semiconductor materials. However, most of the reported 2D chiral perovskites have limited structural types and contain high levels of toxic lead, which severely hinders their further applications. Herein, by using a mixed-cation strategy, an unprecedented type of lead-free cluster-based 2D chiral hybrid double perovskite derivatives are successfully obtained, [( R / S -PPA) 4 (IPA) 6 Ag 2 Bi 4 I 24 ]·2H 2 O ( 1-R and 1-S ), and [( R / S -PPA) 4 ( n -BA) 6 Ag 2 Bi 4 I 24 ]·2H 2 O ( 2-R and 2-S ) ( R / S -PPA= R / S –1-phenylpropylamine; IPA=isopentylamine; n -BA= n -butylamine). Their inorganic skeletons are linked by binuclear {Bi 2 I 10 } and infinite chain {Ag 2 Bi 2 I 14 } ∞ , in which bismuth clusters and multiple coordination modes (e.g., tetrahedral AgI 4 and octahedral AgI 6 ) are introduced into the double perovskite system for the first time. This introduction induces distortion of the inorganic layer, which may facilitate the transfer of chirality from the chiral cations into achiral double perovskite skeletons. Further, circular dichroism measurements and circularly polarized light detection confirm their inherent chiral optical activities. In addition, 1-S exhibits an ultralow X-ray detection limit of 129.5 nGy s −1 , which is 42-fold lower than that of demands in regular medical diagnosis (5.5 µGy s −1 ). This study provides a pathway to construct novel type of lead-free cluster-based double perovskite derivatives.
研究领域:
材料科学
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光学
·
辐射检测
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Ming Ge,Jialu Huang,Yuan Tian,Luozeng Zhou,Han Li,Aichuang Zhang,Sheng Zhu,Xiaorong Zhu,Qiaoxia Li,Yulin Min,Qunjie Xu,Xiaolei Yuan
Carbon-supported Pd-based clusters are one of the most promising anodic catalysts for ethanol oxidation reaction (EOR) due to their encouraging activity and practical applications. However, unclear growth mechanism of Pd-based clusters on the carbon-based materials has hindered their extensive applications. Herein, we first introduce multi-void spherical PdBi cluster/carbon cloth (PdBi/CC) composites by an electrodeposition routine. The growth mechanism of PdBi clusters on the CC supports has been systemically investigated by evaluating the selected samples and tuning their compositions, which involve the big difference in standard redox potential between Pd2+/Pd and Bi3+/Bi and easy adsorption of Bi3+ on the surface of Pd-rich seeds. Benefitting from the ensembles of many nanocrystal subunits, multi-void spherical PdBi clusters can present collective properties and novel functionalities. In addition, the outstanding characteristics of CC supports enable PdBi clusters with stable nanostructures. Thanks to the unique structure, Pd20Bi/CC catalysts manifest higher EOR activity and better stability compared to Pd/CC. Systematic characterizations and a series of CO poisoning tests further confirm that the dramatically enhanced EOR activity and stability can be attributed to the incorporation of Bi species and the strong coupling of the structure between PdBi clusters and CC supports.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganics
·
2025
·Vol. 13
·期 5
·153
·
IF 3
Qianhong Zheng,Genying Zeng,Chenxing Liao,Huoming Huang,Weixiong You,Xinyu Ye,Liaolin Zhang
Bi-doped glasses and fibers have been widely applied in solid-state and fiber lasers. However, the mechanism underlying near-infrared (NIR) luminescence remains unclear, and Bi-related luminescence centers (BLCs) are prone to alteration during fiber fabrication, making it challenging to achieve high-performance Bi-doped glass fibers. In this work, Bi-, Bi-Al-, and Bi-Ge-doped silica glasses were investigated to elucidate the origin of NIR luminescence. Two broad NIR fluorescence bands were observed in silica glasses, originating from distinct BLCs. The longer-wavelength fluorescence band at 1423 nm, demonstrating sensitivity to Bi doping concentration and homogeneity, is attributed to Bi clusters (aggregates of Bi+ions), whereas the shorter-wavelength emission, independent of Bi concentration, originates from isolated Bi+ions. A vacuum-assisted melting-in-tube method with a single-step heating process was employed to fabricate Bi-doped silica-based glasses and fibers. The fluorescence bands of the fibers remained consistent with those of the precursor glasses, indicating no new BLCs were formed during fiber fabrication. The modulation of fluorescence bands was primarily governed by Bi cluster formation. Suppressing Bi clustering through co-doping with Al/Ge or optimizing fabrication conditions offers an effective route to tailor the fluorescence properties of Bi-doped glasses and fibers.
研究领域:
材料科学
·
光学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）