INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Shanshan Wu,Meng Tian,Yang Hu,Nan Zhang,Wei Shen,Jianyi Li,Linchuan Guo,Pengfei Da,Pinxian Xi,Chun-Hua Yan
Formate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO2 modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Huawang Zhao,Yuxin Xie,Bihong Lv,Guohua Jing,Yongdan Li
The CO 2 electrochemical reduction reactions (CO 2 ER) to produce high-value formate are crucial for closing the anthropogenic CO 2 cycle. Modulating the adsorption energy between *OCHO and Bi atoms in Bi-based catalysts could enhance both the activity and selectivity for formate formation. Here, a Bi/BiOBr nanosheet with highly dispersed Bi single atoms in intercalations was synthesized through NaBH 4 treatment of BiOBr, which retained the intercalated Bi atoms after electrolysis (Bi/BiOBr-D). The intercalated Bi atoms optimize the Bi-6p band center (0.016 eV) and charge distribution in Bi/BiOBr-D, enhancing the coupling between the O-2p orbitals of *OCHO and the Bi-6p orbitals as well as the electron transfer dynamics between Bi and the *OCHO intermediate, which improves the stability of the *OCHO intermediate during CO 2 ER. Further studies demonstrate that enhanced *OCHO adsorption reduces the Gibbs free energy barrier for the CO 2 →*OCHO process and suppressing the formation of the *H intermediate. Those advantages lead to high selectivity (FE of 96.83 %) in H-type cell, and excellent activity (j HCOO- of 815 mA/cm²) and productivity (15.22 mmol/h·cm²) in flow cell for formate production over Bi/BiOBr-D sample.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
COMBUSTION AND FLAME
·
2020
·
IF 4.57
Geyuan Yin,Qunfei Gao,Erjiang Hu,Jiawei Xu,Meng Zhou,Zuohua Huang
Laminar flame speeds of formic acid were measured at equivalence ratios of 0.4–1.6, initial temperature of 423–453 K and atmospheric pressure. Chemical kinetic models (Glarborg model and AramcoMech 3.0) were validated against the present experimental data. Deep kinetic insight was investigated using the present models. In addition, detailed analysis was carried out according to transport, thermal and kinetic effect to find out the totally different performance of these two models. The results show that the simulated laminar flame speeds using Glarborg model match well with experimental data while AramcoMech 3.0 apparently over predicts the laminar flame speeds. HOCO and OCHO are driving species for the laminar flame speed of formic acid. Furthermore, the pathway analysis indicates formic acid is consumed mainly by abstraction reaction with OH, forming OCHO radical, which quickly dissociates to H+CO 2 .
研究领域:
燃烧学
·
化学动力学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 9
·4477-4487
·
IF 6.7
Meng Tian,Shanshan Wu,Yang Hu,Zhaori Mu,Zhi Li,Yichao Hou,Pinxian Xi,Chun-Hua Yan
Electrocatalytic reduction of CO2 to formate is considered as a promising method to achieve carbon neutrality, and the introduction of heteroatoms is an effective strategy to improve the catalytic activity and selectivity of catalysts. However, the structural reconstruction behavior of catalysts driven by voltage is usually ignored. Therefore, we used Cu/Bi2S3 as a model to reveal the dynamic reduction process in different atmospheric environments. The catalyst showed an outstanding faradaic efficiency of 94% for formate and a long-term stability of 100 h, and exhibited a high current density of 280 mA cm−2 in a flow cell. The experimental results and theoretical calculations show that the introduction of copper enhances the adsorption of CO2, accelerates the charge transfer and reduces the formation barrier of *OCHO, thus promoting the formation of formate. This work draws attention to the effects of saturated gases in the electrolyte during structural evolution and provides a possibility for designing catalysts with high catalytic activity.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Long Cheng,Rong Wang,Ya Wang,Xingxia Yang,Yanxi Deng,Junhua Li
Formic acid (HCOOH) production from direct CO 2 electrolysis is suggested to be one of the most economically viable products. However, its commercial viability remains challenging in highly active and selective electrocatalysts. Here, we report that palladium (Pd) doping has a profound positive impact on the electrocatalytic activity of bismuth oxide (Bi 2 O 3 ). The introduction of Pd increases the current density and Faradaic efficiency of HCOOH (FE HCOOH ) in flow cell system. As a result, the optimized Pd-Bi catalyst exhibits a FE HCOOH of 99.1 % at −0.7 (V vs RHE). Operating experimental studies coupled with theoretical calculations reveal that the Pd modified active sites exhibit near-optimal binding energy for the key *OCHO intermediate, which is more conducive to the generation of formic acid. Furthermore, the use of an asymmetric low-frequency pulsed strategy stabilizes the active sites, ensuring sustained catalytic performance. This study highlights the potential of Pd-doped Bi 2 O 3 as a promising candidate for efficient and selective CO 2 electroreduction to formic acid.
研究领域:
催化化学
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电化学
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环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Xin Li,Jun-Hao Wang,Chen-Yue Yuan,Qi-Wen Sun,Jiang Shao,Xing-Chi Li,Zhao-Lu Feng,Hao Dong,Chen Li,Ya-Wen Zhang
The CO 2 electroreduction reaction using sustainable electricity emerges as a viable strategy to produce high-value-added and profitable chemicals. The achievement of superior activity at a lower overpotential and higher selectivity in a wide potential window is vitally important for large-scale industrial applications. Herein, a carbon-composite amorphous porous BiSbO x nanotube with abundant unsaturated sites is reported to boost the conversion of CO 2 to formate, exhibiting a formate selectivity of >90% in an extremely broad range of potentials from −0.5 to −1.4 V versus reversible hydrogen electrode (RHE) and a maximal energy conversion efficiency of 77.1%. Importantly, pure formic acid solution is directly obtained in a solid-electrolyte cell for industrial-scale applications. The porous tubular structure can expose more catalytic active sites, accelerate the mass transfer, and show fast surface charge transfer. Moreover, the unique coordination-unsaturated Sb-stabilized BiO 8−x site can not only enhance the adsorption and activation of CO 2 but also reasonably balance the stabilization and hydrogenation of *OCHO intermediate, thus leading to its obviously higher catalytic performance. As a result, a novel amorphous porous BiSbO x nanotube is successfully designed for efficient CO 2 electroreduction, which may shed new light on developing many more amorphous composite metal oxide catalysts for conversion of inert small molecules.
研究领域:
电化学
·
纳米材料
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催化
·
材料科学
·
能量转换
✓ 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）