Nature Communications
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2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Tang Yulong,Li Jiejie,Lin Yichao,Cheng Moxing,Wang Shuibo,Tian Ziqi,Zhou Junjie,Zhang Haolei,Wang Yunan,Chen Liang
The electrochemical reduction of acetonitrile (AN) to ethylamine (EA) is an attractive yet challenging process, primarily due to the competing hydrogen evolution reaction (HER). This study demonstrates the ability to halt the HER at Volmer step, where protons migrate to the unsaturated bond of AN on a self-supported CuO@Cu heterostructure. The CuO@Cu catalyst exhibits nearly 100% Faradaic efficiency (FE) over the entire range of potentials tested from −0.1 to −0.4 V vs. RHE, demonstrating remarkable stability over 1000 h at a constant current density of 0.2 A cm −2 . CuO is identified as the active component driving the reaction, while the metallic Cu facilitates efficient electron transfer. Theoretical simulations and experimental evidences indicate that a synergistic hydrogenation process contributes to the AN reduction reaction (ARR), which involves both surface hydrogen migration and proton addition from solution. This study provides an insight into understanding of ARR process, and suggests an efficient strategy to enhance the electrochemical hydrogenation of organic molecules by regulating the Volmer step.
研究领域:
电化学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL PHYSICS
·
2020
·Vol. 33
·期 3
·296-302
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IF 1.067
Zhang Hang,Li Yan-bo,Zhu Long,Chen Jun,Yu Ye-peng,Li Zhao-hui,Lin Xuan,Shan Xiao-bin,Liu Fu-yi,Sheng Liu-si
Vacuum ultraviolet (VUV) photoionization and photodissociation of methylcyclohexane have been studied utilizing a reflectron time-of-flight mass spectrometer (RTOF-MS) with synchrotron radiation source. Photoionization efficiency curves (PIEs) of molecule ion C 7 H 14 + and fragment ions C 7 H 13 + , C 6 H 11 + , C 6 H 10 + , C 5 H 10 + , C 5 H 9 + , C 4 H 8 + , C 4 H 7 + , and C 3 H 5 + were observed. The ionization energy of methylcyclohexane was measured to be (9.80±0.03) eV, and appearance energies of fragment ions were determined from the PIEs. Optimized structures of transitional states, intermediates and product ions were characterized at the B3LYP/6-31G(d) level and the energies were calculated using G3B3 method. Formation channels of dominating fragment ions were proposed. Intramolecular hydrogen migrations and carbon ring-opening were the foremost processes in fragmentation pathways of methylcyclohexane.
研究领域:
物理化学
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分子光谱学
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Guang-Hui Liu,Jin-Jun Bai,Kun-Lang Lu,Hui Kan,Xiao-Qi Zhang,Yu-Hong Kang,Cui-Ying Lu,Zhan-Ku Li,Hong-Cun Bai,Xian-Yong Wei
Two flexible regulation systems were designed and used for the integrated catalytic hydroconversion (CHC) of lignocellulose to valuable oxygenated organic chemicals. Under the dual constraints of initial H 2 pressure (IHP) and temperature, three crop stalks can be almost completely degraded over a hydrothermally stable Ru/La(OH) 3 in one-pot, while the synergetic transfer of active hydrogen effectively promotes the cleavage of >C-O- bridged bonds in organic matter with highly complex structures during this period. As a result, abundant >C al -O- (>32%) and >C=O (>24%) derived platform chemicals such as alkanols, cyclanols, carboxylic acids, and esters were obtained at high IHP and low temperature. Correspondingly, various >C ar -O- (>50%) and >C=O (>30%) derived platform chemicals such as phenols, alkoxy-substituted phenols, ketones, and carboxylic acids dominated the derived bio-oils at low IHP and high temperature. The designed selective CHC strategies have the characteristics of convergent conversion to the two major derivative chemical demand directions. Therefore, these two atom-economic and effective degradation approaches are conducive to obtaining abundant functional small molecules, which can be further converted to various downstream platform products.
研究领域:
化学工程
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生物质能
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催化科学
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
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2025
·
IF 6.7
Jinjuan Zhao,Sizhuo Ma,Dan Huang,Jie Wu,Zheng Liu,Mengjie Li,Honglei Yang,Shuwen Li
Hydrogen spillover, involving the migration of hydrogen species produced by ethanol oxidation from metal nanoparticles to support materials, is conductive to develop advanced electrocatalysts applicable to ethanol oxidation reaction (EOR) and further overcome the performance limitations. Herein, the ethylenediamine-modified C 60 (AC 60 ) embedded in nitrogen-doped graphene aerogel (NG) anchoring Pd nanocrystals (Pd/AC 60 @NG) was synthesized as an electrocatalyst for EOR. The high curvature of C 60 with the partial localization of p electrons and the increase of sp 3 characteristics is of great significance for enhancing the interaction with hydrogen species and accelerating the migration of hydrogen species from the Pd surface to the C 60 surface. Due to highly delocalized π-sphere surface, excellent electron nucleophilicity and minimal reorganization energy requirements, C 60 can generate powerful electron and space confinement effects to hasten electron transfer and mitigate Ostwald ripening process. The intense interaction is established between C 60 and NG through strong hydrogen bonds after C 60 is modified by ethylenediamine, which enhances the stability and dispersibility of C 60 . The prepared Pd/AC 60 @NG exhibited significantly improved electrocatalytic activity compared to commercial Pd/C. This study opens new possibilities for designing and developing new carbon-based materials aimed at enhancing catalytic activity for ethanol oxidation, hydrogen evolution, and the oxygen reduction reaction.
研究领域:
电化学
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催化
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纳米材料
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能量转换
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hongbing Wang,Yifei Yang,Shixiang Yu,Beibei Zhang,Junzhong Xie,Jun Chen,Dongping Wang,Bomin Feng,Changyin Zhong,Linsen Zhou,Wei Cui,Ding Ma,Yunxi Yao
Liquid-phase hydrogen isotopes exchange between hydrogen and water is a promising route for the hydrogen isotopes separation from water, catalyzed by the metal Pt with hydrophobic coating to surmount the flooding of reactive sites. However, poor water activation ability on Pt has limited the catalytic efficiency of Pt-based catalysts and hindered their application. Herein, we report a bifunctional Pt/ZSM-5 catalyst with hydrophobic modification by surface silylation for H 2 -HDO isotope catalytic exchange. The integration of metallic Pt and Brønsted acid (BA) sites in the microporous ZSM-5 boosts the catalytic efficiency of deuterium extraction by two orders of magnitude compared to commercial Pt-C at the optimum condition. In-situ spectroscopic and theoretical studies demonstrated that HDO-H 2 O preferentially adsorbs on BA sites (-Si-OH-Al) to form protonated water clusters stabilized by hydrogen-bonded network or to undergo the proton exchange to leave deuterium on zeolite framework as a new acidic site ([AlO 4 D]). Under the attractive interaction, the dissociated hydrogen on Pt clusters releases partial electrons to form positively-charged hydrogen, which further transfers to the [AlO 4 D] sites or protonated water clusters by interfacial spillover to produce the overcharging intermediates. These intermediates cleave their O-D bonds to form positively charged D, which ultimately spills back to Pt cluster and combines with the remaining electron to desorb in the form of HD. The synergistic effect between Pt and BA sites creates a new pathway of hydrogen transfer, which enables the more efficient hydrogen-water isotope exchange on the bifunctional Pt/ZSM-5 catalyst.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
DOI
高影响因子
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