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Molecule aging induced by electron attacking 认领 引用
1
作者 Ping Song Yining Dong +5 位作者 Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期519-525,I0013,共7页
Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"... Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H2O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H2O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications. 展开更多
关键词 Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction
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Steering CO2electrolysis selectivity by modulating the local reaction environment:An online DEMS approach for Cu electrodes 认领 引用 被引量：6
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作者 Ke Ye Guiru Zhang +6 位作者 Baoxin Ni Liang Guo Chengwei Deng Xiaodong Zhuang Changying Zhao Wen-Bin Cai Kun Jiang 《eScience》 2023年第4期89-98,共10页
Electrochemical CO2reduction is a typical surface-mediated reaction,with its reaction kinetics and product distributions largely dependent on the dynamic evolution of reactive species at the cathode–catholyte inte... Electrochemical CO2reduction is a typical surface-mediated reaction,with its reaction kinetics and product distributions largely dependent on the dynamic evolution of reactive species at the cathode–catholyte interface and on the resultant mass transport within the hydrodynamic boundary layer in the vicinity of the cathode.To resolve the complex local reaction environment of branching CO2reduction pathways,we here present a dif-ferential electrochemical mass spectroscopic(DEMS)approach for Cu electrodes to investigate CO2mass trans-port,the local concentration gradients of buffering anions,and the Cu surface topology effects on CO2electrolysis selectivity at a temporal resolution of~400 ms.As a proof of concept,these tuning knobs were validated on an anion exchange membrane electrolyzer,which delivered a Faradaic efficiency of up to 40.4%and a partial current density of 121 mA cm-2for CO2-to-C2H4valorization.This methodology,which bridges the study of fundamental surface electrochemistry and the upgrading of practical electrolyzer performance,could be of general interest in helping to achieve a sustainable circular carbon economy. 展开更多
关键词 Spectroelectrochemistry CO2reduction reaction Copper electrode Differential electrochemical mass spectroscopy Local reaction environment
Artificial synthesis of polyesters at ambient condition via consecutive CO2electrolysis and fermentation 认领 引用 被引量：3
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作者 Guiru Zhang Ning Ji +9 位作者 Shiheng Lyu Baoxin Ni Peng Shen Ke Ye Yuting Wang Xuheng Jiang Hai Zhang Xi Liu Yongcheng Wang Kun Jiang 《Nano Research》 SCIE EI CSCD 2024年第7期6016-6025,共10页
Electrochemically converting CO2into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions,yet largely limited to short-chained C1–C3products.Herein,we demonstrate a tandem... Electrochemically converting CO2into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions,yet largely limited to short-chained C1–C3products.Herein,we demonstrate a tandem artificial synthesis of biodegradable polyhydroxybutyrate(PHB)plastic from CO2building blocks.Batch synthesis of defects-enriched Bi catalyst is firstly demonstrated by plasma bombardment and following in situ electrochemical reduction,which delivers a HCOOH Faradaic efficiency above 80%at tunable concentration from 2 to 250 mM,an energy efficiency up to 41%,and a single-pass carbon conversion efficiency up to 60%.Annular dark field and second electron microscopic analysis,density functional theory(DFT)calcualtions,coupled with H-type and solid-state electrolyzer assessments,point out the vital role of defective and/or stepped Bi surface sites in promoting CO2-to-HCOOH conversion.Thereafter,as-synthesized high-purity HCOOH is used as the sole carbon source for C-chain growth within microbial fermentation reactor with Ralstonia eutropha,where activated formate dehydrogenase and increased metabolites related to Calvin–Benson–Bassham cycle are found to be responsible for the enhanced polyester accumulation. 展开更多
关键词 CO2electrolysis Bi catalyst vacancy site formic acid fermentation
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Thin-Layer Diamond Coating on Si Wafer for Extended Alkaline ATR-SEIRAS Investigations 认领 引用
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作者 Wencheng Li Wei-Yi Zhang +6 位作者 Baoxin Ni Peng Shen Yu Qiao Xinchang Wang Xian-Yin Ma Wen-Bin Cai Kun Jiang 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2024年第23期3063-3068,共6页
Electrochemical attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)plays an important role in deciphering interfacial reaction mechanisms at molecular level.However,the corrosive ... Electrochemical attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)plays an important role in deciphering interfacial reaction mechanisms at molecular level.However,the corrosive etching of Si internal reflection element by OH−largely impedes reliable SEIRAS measurements in strong alkaline electrolytes.Herein,a dense and chemically inert nanocrystalline diamond(NCD)film is successfully fabricated at a thickness of~120 nm through hot filament chemical vapor deposition on a micromachined Si wafer to insulate the OH−etching.A reversible interfacial water feature without spectral interference of Si-O band is obtained in 1.0 mol·L–1KOH on Au/NCD/Si film electrode.Afterwards,electrochemical CO reduction reaction on Cu film electrode is explored in different KOH concentrations ranging from 0.1 to 3.0 mol·L-1as a model reaction.A redshift of COLband,as well as its lower intensity but faster depletion kinetics,is noted with increasing electrolyte pH,whereas COBis identified as an inert spectator accumulating on Cu surface.Our present work demonstrates the alkaline resistant feature of diamond/Si composite internal reflection element,which could be a powerful platform to study electrocatalytic reactions in strong alkaline media. 展开更多
关键词 Electrochemistry Electrocatalysis ATR-SEIRAS Thin-layer diamond Strong alkaline Micromachined Si IR spectroscopy
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