催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
11期
1833-1839
,共7页
齐随涛%李迎迎%岳佳琪%陈昊%伊春海%杨伯伦
齊隨濤%李迎迎%嶽佳琪%陳昊%伊春海%楊伯倫
제수도%리영영%악가기%진호%이춘해%양백륜
铂%镍%双金属%十氢化萘%脱氢%密度泛函理论
鉑%鎳%雙金屬%十氫化萘%脫氫%密度汎函理論
박%얼%쌍금속%십경화내%탈경%밀도범함이론
Platinum%Nickel%Bimetallic%Decalin%Dehydrogenation%Density functional theory
采用等体积浸渍法制备了活性炭负载的具有脱氢活性的Pt-Ni双金属催化剂及相应的Pt单金属催化剂,并用X射线衍射、N2吸附-脱附和NH3-程序升温脱附对其进行了表征。在290°C下,研究了间歇反应条件下催化剂以过热液膜状态催化十氢化萘脱氢活性,考察了温度、浸渍顺序和Pt/Ni摩尔比对十氢化萘脱氢活性和萘产率的影响。结果表明,与单金属催化剂相比, Pt-Ni双金属催化剂上产氢效率显著提高。当Pt/Ni摩尔比为1:1, Pt首先浸渍时,得到的催化剂上脱氢转化率和萘产率最高。将实验结果与密度泛函理论计算的氢原子在不同催化表面的结合能关联证实,具有更强原子氢结合能的双金属表面具有更高的脱氢活性。
採用等體積浸漬法製備瞭活性炭負載的具有脫氫活性的Pt-Ni雙金屬催化劑及相應的Pt單金屬催化劑,併用X射線衍射、N2吸附-脫附和NH3-程序升溫脫附對其進行瞭錶徵。在290°C下,研究瞭間歇反應條件下催化劑以過熱液膜狀態催化十氫化萘脫氫活性,攷察瞭溫度、浸漬順序和Pt/Ni摩爾比對十氫化萘脫氫活性和萘產率的影響。結果錶明,與單金屬催化劑相比, Pt-Ni雙金屬催化劑上產氫效率顯著提高。噹Pt/Ni摩爾比為1:1, Pt首先浸漬時,得到的催化劑上脫氫轉化率和萘產率最高。將實驗結果與密度汎函理論計算的氫原子在不同催化錶麵的結閤能關聯證實,具有更彊原子氫結閤能的雙金屬錶麵具有更高的脫氫活性。
채용등체적침지법제비료활성탄부재적구유탈경활성적Pt-Ni쌍금속최화제급상응적Pt단금속최화제,병용X사선연사、N2흡부-탈부화NH3-정서승온탈부대기진행료표정。재290°C하,연구료간헐반응조건하최화제이과열액막상태최화십경화내탈경활성,고찰료온도、침지순서화Pt/Ni마이비대십경화내탈경활성화내산솔적영향。결과표명,여단금속최화제상비, Pt-Ni쌍금속최화제상산경효솔현저제고。당Pt/Ni마이비위1:1, Pt수선침지시,득도적최화제상탈경전화솔화내산솔최고。장실험결과여밀도범함이론계산적경원자재불동최화표면적결합능관련증실,구유경강원자경결합능적쌍금속표면구유경고적탈경활성。
Pt-Ni bimetallic catalysts and the corresponding monometallic Pt catalysts supported on active carbon were prepared by incipient wetness impregnation and characterized by X-ray diffraction, N2 adsorption, and NH3-temperature programmed desorption. Their activities for decalin dehydro-genation were investigated at a superheated liquid film state in a batch reactor. The effects of tem-perature, impregnation sequence, and Pt/Ni molar ratio on the dehydrogenation activity and the naphthalene yield were investigated. The results show that the Pt-Ni bimetallic catalyst significantly enhanced hydrogen evolution compared with either Ni or Pt monometallic catalyst. The highest dehydrogenation conversion and naphthalene yield were obtained when the Pt/Ni molar ratio was 1:1 and Pt was impregnated first. The experimental results were correlated with density functional theory calculations of hydrogen binding energy (HBE) on different catalytic surfaces. The correla-tion confirmed that bimetallic surfaces with stronger HBEs had higher dehydrogenation activities.