化学反应工程与工艺
化學反應工程與工藝
화학반응공정여공예
Chemical Reaction Engineering and Technology
2015年
4期
352-358
,共7页
王琴%王晓春%杨冬伟%李露%贾友见%施锦
王琴%王曉春%楊鼕偉%李露%賈友見%施錦
왕금%왕효춘%양동위%리로%가우견%시금
二氧化碳%电化学还原%中毒机理%电极失活
二氧化碳%電化學還原%中毒機理%電極失活
이양화탄%전화학환원%중독궤리%전겁실활
carbon dioxide%electrochemistry reduction%poisoning mechanism%electrode deactivation
在水溶液中,电还原CO2制取CO时,电极易中毒失活,采用扫描电子显微镜(SEM)、X 射线光电子能谱(XPS)对反应前后的电极材料进行检测,研究CO2在KHCO3水溶液中发生电化学还原反应时,Au电极失活原因及电极材料活性降低对反应过程的影响.结果表明,电极表面吸附了一层黑色有害物质.这层黑色有害物质大部分是石墨碳,并有微量的铁和锌.采用塔菲尔曲线、电化学阻抗(EIS)、线性扫描曲线、恒电位电解和气相色谱法等研究了有害物质对CO2电还原反应动力学过程的影响,发现随着反应的进行,生成CO的平衡电位负移,电荷转移电阻增大,交换电流密度变小,产物CO的电流效率迅速降低.说明电极表面附着的有害物质使电极材料活性降低,阻碍了CO2电还原反应的进行.
在水溶液中,電還原CO2製取CO時,電極易中毒失活,採用掃描電子顯微鏡(SEM)、X 射線光電子能譜(XPS)對反應前後的電極材料進行檢測,研究CO2在KHCO3水溶液中髮生電化學還原反應時,Au電極失活原因及電極材料活性降低對反應過程的影響.結果錶明,電極錶麵吸附瞭一層黑色有害物質.這層黑色有害物質大部分是石墨碳,併有微量的鐵和鋅.採用塔菲爾麯線、電化學阻抗(EIS)、線性掃描麯線、恆電位電解和氣相色譜法等研究瞭有害物質對CO2電還原反應動力學過程的影響,髮現隨著反應的進行,生成CO的平衡電位負移,電荷轉移電阻增大,交換電流密度變小,產物CO的電流效率迅速降低.說明電極錶麵附著的有害物質使電極材料活性降低,阻礙瞭CO2電還原反應的進行.
재수용액중,전환원CO2제취CO시,전겁역중독실활,채용소묘전자현미경(SEM)、X 사선광전자능보(XPS)대반응전후적전겁재료진행검측,연구CO2재KHCO3수용액중발생전화학환원반응시,Au전겁실활원인급전겁재료활성강저대반응과정적영향.결과표명,전겁표면흡부료일층흑색유해물질.저층흑색유해물질대부분시석묵탄,병유미량적철화자.채용탑비이곡선、전화학조항(EIS)、선성소묘곡선、항전위전해화기상색보법등연구료유해물질대CO2전환원반응동역학과정적영향,발현수착반응적진행,생성CO적평형전위부이,전하전이전조증대,교환전류밀도변소,산물CO적전류효솔신속강저.설명전겁표면부착적유해물질사전겁재료활성강저,조애료CO2전환원반응적진행.
The working electrode might get inactivate easily in the process of electrochemical reduction of CO2 to CO in aqueous solution. The effects of the deactivation reasons of the Au electrode and the decrease of electrode activity on the reaction during the electrochemical reduction of CO2 in KHCO3 aqueous solution, and the surface of Au electrode were investigated by scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS).The results showed that a small amount of impurities composed of C graphite and a little of Fe and Zn adsorbed on the surface of the Au electrode. The electrochemical kinetic characteristics of CO2 reduction on Au electrode were studied using Tafel curve, Electrochemical impedance spectroscopy(EIS), Linear sweep curve, Potentiostatic electrolysis, and gas chromatographic. As a result, with the reaction going on, the equilibrium potential of CO2 conversion to CO shifted to negative, the electron transfer resistance rised up, the exchange current density reduced continuously, and the faradaic efficiency of CO decreased rapidly, which indicated that C graphite and metal adsorbed on the electrode decreased the electrocatalytic activity of Au electrode, and hindered the CO2 reduction.