CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zhiqin Deng,Jie Liang,Qian Liu,Chaoqun Ma,Lisi Xie,Luchao Yue,Yuchun Ren,Tingshuai Li,Yongsong Luo,Na Li,Bo Tang,Abdulmohsen Ali Alshehri,Imran Shakir,Philips O. Agboola,Shihai Yan,Baozhan Zheng,Juan Du,Qingquan Kong,Xuping Sun
A Co 2 AlO 4 nanosheet array on carbon cloth (Co 2 AlO 4 /CC) is proposed as a superb electrocatalyst for converting nitrate (NO 3 − ) to ammonia (NH 3 ). In 0.1 M PBS solution with 0.1 M NO 3 − , it attains an NH 3 yield of 7.9 mg h −1 cm −2 with a Faradaic efficiency of 92.6%, with high durability. A Zn-NO 3 − battery with such Co 2 AlO 4 /CC as cathode offers a power density of 3.43 mW cm −2 with an NH 3 yield of 750 μg h −1 cm −2 . Theoretical calculations reveal that Al ions reduce the electron cloud density on the surface of Co, making it highly conducive to NO 3 − adsorption at Co sites. Additionally, Co 2 AlO 4 (2 2 0) surface inhibits hydrogen evolution reaction but is highly active for NO 3 − reduction with a low energetically uphill pathway (ΔG of 0.42 eV) for the potential-determining step (*NO 3 to *NO 3 H), much smaller than that of Co 3 O 4 (2 2 0) (ΔG of 0.83 eV).
研究领域:
材料科学
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电化学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Youqun Chu,Xiaoping Zhang,Xinyu Liu,Hao Tang,Weitao Zhou,Kaiwen Li,Xin Liu,Zhaoyang Chen,Yinghong Zhu,Fengming Zhao
An efficient and mild iodide-mediated indirect electrooxidation method to prepare 2,6-dichlorobenzonitrile was developed. Cyclic voltammetry and potentiostatic electrolysis were carried out to investigate the feasibility of this approach for 2,6-dichlorobenzaldehyde. Unexpectedly, an increase in the synthetic efficiency was obtained when the solution contained chloride ions. The cyclic voltammetric results indicated that an interhalide species, namely [ICl 2 ] − , was formed during oxidation of the iodide ion in the solutions containing chloride ions; this result was in contrast to the expected formation of the less electrophilic I 2 . The strong electrophilicity of [ICl 2 ] − greatly enhanced the efficiency of the electrosynthetic approach to 2,6-dichlorobenzonitrile. Overall, this synthesis system provides a green and efficient route to 2,6-dichlorobenzonitrile, and hence, could be potentially applicable in the industrial preparation of aromatic nitriles.
研究领域:
有机化学
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电化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Guanqing Ding,Changlong Li,Wendong Liu,Xiaoxue Zhao,Yuanyuan Jiang,Yizhong Lu
Electrochemical oxygen reduction reaction (ORR) via two-electron pathway is a viable method to produce hydrogen peroxide (H 2 O 2 ). Here, oxidized carbon nanotubes (O-CNTs) rich in oxidized functional groups are obtained by rapid kneading oxidation within two hours. The optimal sample, O-CNTs-7, exhibits remarkable electrocatalytic performance for the H 2 O 2 production under alkaline environment. The O-CNTs-7 shows a high onset potential of 0.74 V (vs. RHE), and could delivers up to 90% selectivity for H 2 O 2 production over a wide voltage window (0.3 V to 0.7 V). In situ attenuated total reflection infrared (ATR-IR) spectroscopy show the certain relationship between potential and the adsorption behavior of *HOOH and *OOH, which confirm the associative two-electron pathway for O-CNTs-7. This study provides a general method to obtain highly oxidized carbon materials with abundant oxygen-containing groups towards highly efficient H 2 O 2 electrosynthesis.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ACS Catalysis
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2023
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IF 12.9
Yingying Cheng,Wenjing Xu,Jing Hou,Peng Kang
The electrosynthesis of multi-carbon chemicals such as glyoxylic acid (GX) and glycolic acid (GC) from oxalic acid (OA) offers a feasible pathway to achieve sustainable chemical production, especially when coupled with the electroreduction of CO2 to form OA. Here, we demonstrate a series of gallium tin oxide catalysts for selective, controlled OA electroreduction to GX and GC in acidic media. The product distribution can be tuned by changing the reaction temperatures. At room temperature using the GaSnOx/C catalyst, GX can be obtained with a GX Faradaic efficiency (FEGX) of 92.7% at −0.7 V vs RHE and a GX current density (jGX) of −100.2 mA cm–2. At a raised temperature of 80 °C using the GaSnOx/C catalyst, a GC Faradaic efficiency (FEGC) of 91.7% at −0.8 V vs RHE can be obtained. The accelerated OA electroreduction results from the Ga/Sn synergy in the catalysts. A proper Ga/Sn ratio not only enriches OA adsorption and enhances surface binding of intermediates, but also ensures catalyst stability in acidic media.
研究领域:
化学工程
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材料科学
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可持续化学
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DOI
高影响因子
Inorganics
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2023
·Vol. 11
·期 9
·349
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IF 2.9
Xinyi Zhou,Yang-Rong Yao,Yajing Hu,Le Yang,Shaoting Yang,Yilu Zhang,Qianyan Zhang,Ping Peng,Peng Jin,Fang-Fang Li
The reactivity of the open-shell Gd@C2v-C82with different charge states towards benzyl bromide was investigated. [Gd@C2v-C82]3−exhibited enhanced activity relative to Gd@C2v-C82and [Gd@C2v-C82]−. The structural characterizations, including MALDI-TOF MS, UV-vis-NIR, and single crystal X-ray diffraction, indicate the formation of isomeric benzyl monoadducts of Gd@C2v-C82. All three monoadducts contain 1:1 mirror-symmetric enantiomers. Additionally, the addition of the benzyl group and its specific position result in distinct electrochemical behavior of the products compared to the parent Gd@C2v-C82. Theoretical studies demonstrate that only [Gd@C2v-C82]3−has a HOMO energy level that matches well with the LUMO energy level of the PhCH2radical, providing a rationalization for the observed significantly different reactivity.Keywords:endohedral metallofullerene;open shell;electrosynthesis;fullerene anion;Gd@C2v-C82
研究领域:
化学
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材料科学
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DOI
高影响因子
ACS Omega
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2023
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IF 4.1
Kun Luo,Ya Li,Tong Liu,Xiangqun Zhuge,Etelka Chung,Andrew R. Timms,Simon P. Graham,Guogang Ren
Copper nanoparticles (CuNPs) and gold nanoclusters (AuNCs) show a high catalytic performance in generating hydrogen peroxide (H2O2), a property that can be exploited to kill disease-causing microbes and to carry carbon-free energy. Some combinations of NPs/NCs can generate synergistic effects to produce stronger antiseptics, such as H2O2 or other reactive oxygen species (ROS). Herein, we demonstrate a novel facile AuNC surface decoration method on the surfaces of CuNPs using galvanic displacement. The Cu–Au bimetallic NPs presented a high selective production of H2O2 via a two-electron (2e–) oxygen reduction reaction (ORR). Their physicochemical analyses were conducted by scanning electron microscopy (SEM), transmitting electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). With the optimized Cu–Au1.5NPs showing their particle sizes averaged in 53.8 nm, their electrochemical analysis indicated that the pristine AuNC structure exhibited the highest 2e– selectivity in ORR, the CuNPs presented the weakest 2e– selectivity, and the optimized Cu–Au1.5NPs exhibited a high 2e– selectivity of 95% for H2O2 production, along with excellent catalytic activity and durability. The optimized Cu–Au1.5NPs demonstrated a novel pathway to balance the cost and catalytic performance through the appropriate combination of metal NPs/NCs.
研究领域:
材料科学
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生物学
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化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Chen Shu,Bin Chen,Weihu Zhang,Lele Cui,Wenheng Jing
Renewable electricity-driven hydrogen peroxide (H 2 O 2 ) electrosynthesis technology has recently emerged as a multidisciplinary research frontier as its distributed deployment capability can provide enhanced versatility for various potential niche applications. Despite significant progress in screening advanced electrocatalysts and fundamental understanding of microscopic reaction mechanisms, industrially viable electrolysis devices suitable for this technology are still lacking due to technical challenges such as low space/electrode utilisation and single-pass yield as well as poor operability. Here, we demonstrate a membrane-free dual-cathode stack reactor featuring compactness (inter-electrode distance configured to flow field plate thickness) and ideal electrode utilisation (two cathodes paired with one anode). Structurally discontinuous carbon films with self-sustained aeration are assembled as cathodes, which enables open air-fed O 2 -to-H 2 O 2 conversion and thus effectively simplifies operation. Even with low electrolyte concentrations (0.05 M Na 2 SO 4 ), this design demonstrates efficient H 2 O 2 production from bench- to industrial-scale operating current densities (75–200 mA cm −2 ) at relatively low cell voltages (5.9–11.0 V). Impressive single-pass H 2 O 2 accumulations of 959.6–2332.1 mg L −1 with current efficiencies of 55.1 %–90.7 % can be achieved at low hydraulic retention times of 15–60 s. The practicality and reliability of the device can be further elucidated by its robustness in decentralized wastewater remediation scenarios. This all-material/components-commercial design paves the way for advancing the technology readiness level of H 2 O 2 electrosynthesis processes.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Haichuan He,Congcheng Yang,Liu Deng,Li Luo,Yahui Jiang,Liqiang Wang,Yi Zhang,Minghui Yang,You-Nian Liu
CO 2 -to-formate electrosynthesis with high selectivity and stability has been a long-sought objective. Unfortunately, most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage, resulting in decreased catalytic performance. Herein, we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi 0 active sites to renew the surface activation. The electronic structure of Bi site can be regulated by introducing In, thereby enhancing the adsorption strength of *OCHO. The optimized electrode exhibits over 90% FE formate at a wide potential window (−0.9–−2.2 V), and formation rate for 3.15 mM cm −1 h −1 . Especially, the electrode can maintain the high performance at continuously electrolysis for more than 300 h, or for more than 50 cycles, even repeated operation and storage for more than 2 years. This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.
研究领域:
材料科学
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电化学
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能源转化
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产品关联
DOI
高影响因子
Chem Catalysis
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2022
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IF 0
Wenjie Wu,Yulu Yang,Yitong Wang,Tiantian Lu,Qingsong Dong,Junwei Zhao,Jingyang Niu,Qingchao Liu,Zhaomin Hao,Shuyan Song
Electrosynthesis of urea from N 2 and CO 2 molecules is of immense significance but has so far been plagued by the lack of a universal design principle to guide the search for new catalysts. Herein, as exemplified by the Cu-Bi catalyst, our findings revealed that the defective Cu-Bi catalyst could offer a maximum urea concentration of 0.45 ± 0.06 mg L −1 and the largest faradaic efficiency of 8.7% ± 1.7% at −0.4 V (versus reversible hydrogen electrode [RHE]), exhibiting outstanding activity in contrast to monometallic (Cu and Bi) and bimetallic (Cu-Bi mixture and intact Cu-Bi) catalysts. Moreover, the evidence from isotope tracing experiments, in situ Raman spectroscopy, and density functional theory (DFT) calculations suggested that it is a promising strategy for the co-reduction of N 2 and CO 2 by defective Cu-Bi catalysts, switching on a light to the application of defects in electrosynthesis of urea.
研究领域:
化学工程
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材料科学
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催化反应
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DOI
BIOELECTROCHEMISTRY
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2018
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IF 3.789
Shanshan Chen,Yanlun Fang,Xianyue Jing,Hailin Luo,Jing Chen,Shungui Zhou
Microbial electrosynthesis systems (MES) are promising devices in which microbes obtain electrons from electrodes to produce extracellular multicarbon compounds. This study investigates whether improvement in cell permeability can enhance electrosynthesis performance of Gram-positive Moorella thermoautotrophica in MES. Results showed that when ≤30 mg/L penicillin was added, the cell permeability was doubled, and the electron uptake per biomass (including both cathode-associated biomass and suspended biomass) was 1.84 times that of the control, while formate and acetate production rates per biomass were 1.96 and 2.23 times those of the control, respectively. Enhanced cell permeability caused higher redox activities of outmost cytochrome C and increased release of redox electron shuttles, both of which were beneficial to extracellular electron uptake. Coulombic efficiencies increased from 73% ± 3% to 88% ± 3% with better cell permeability, demonstrating that higher proportion of electrical energy recovered in the chemical-production reaction. This research demonstrates that making a moderate decrease in peptidoglycan of cell walls to improve cell permeability can enhance electron uptakes and chemical production rates of Gram-positive microbes in MES, which would serve as a base for the future genetic modification study of superior electrosynthesis strains.
研究领域:
微生物学
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生物技术
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环境科学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
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2023
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IF 17.1
Huitong Du,Li-Xia Liu,Pan Li,Qianhao Min,Shaojun Guo,Wenlei Zhu
Fine-tuned catalysts that alter the diffusion kinetics of reaction intermediates is of great importance for achieving high-performance multicarbon (C2+) product generation in carbon monoxide (CO) reduction. Herein, we conduct a structural design based on Cu2O nanoparticles and present an effective strategy for enhancing propanol electrosynthesis from CO. The electrochemical characterization, operando Raman monitoring, and finite-element method simulations reveal that the multishell structured catalyst can realize the enrichment of C1 and C2 intermediates by nanoconfinement space, leading to the possibility of further coupling. Consequently, the multishell copper catalyst realizes a high Faraday efficiency of 22.22 ± 0.38% toward propanol at the current density of 50 mA cm–2.
研究领域:
化学
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材料科学
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电催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
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2024
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IF 6.1
Zongyi Wang,Jiuli Chang,Zhiyong Gao
Nitrate–methanol co-electrolysis involving the cathodic nitrate reduction reaction (NO3RR) combined with the anodic methanol oxidation reaction (MOR) is a viable way to synchronously produce ammonia (NH3) and formate via gentle, sustainable and energy-saving “E-refining” and “E-reforming” means. An efficient bifunctional catalyst for the NO3RR and MOR is pivotal to achieve such a goal. In this work, a nitrogen-doped carbon-encapsulated nickel iron phosphide hybrid (Ni2FeP@NC) was prepared as a bifunctional catalyst for the NO3RR and MOR, and its electrochemical performance for nitrate–methanol co-electrolysis was investigated. The Ni2FeP@NC catalyst exhibited a high NH3 yield (0.47 mmol h−1 cm−2 at −0.35 V) and faradaic efficiency (FE, 93% at −0.15 V) for the NO3RR and simultaneously demonstrated high MOR efficiency for formate production (yield of 1.62 mmol h−1 cm−2 at 1.7 V and FE of around 95%). The bifunctional catalytic features of the nitrate–methanol co-electrolysis system enabled the concurrent production of NH3 and formate at low input voltage. This work provides a viable paradigm for pairwise electrosynthesis of valuable chemicals via “E-refining” and “E-reforming” through the rational design of bifunctional catalysts.
研究领域:
化学工程
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环境科学
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材料科学
✓ 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）