{"id":189280,"date":"2019-11-25T06:30:33","date_gmt":"2019-11-24T22:30:33","guid":{"rendered":"\/\/m.iemloyee.com\/?p=189280"},"modified":"2019-11-23T21:24:00","modified_gmt":"2019-11-23T13:24:00","slug":"%e3%80%90%e5%b7%b2%e6%a0%a1%e7%a8%bf%e3%80%91jacs%ef%bc%9arh1-mos2%e5%8d%95%e5%8e%9f%e5%ad%90%e5%82%ac%e5%8c%96%e5%89%82%e7%9a%84%e7%b1%bb%e9%85%b6%e5%9b%8a%e7%8a%b6%e6%b4%bb%e6%80%a7%e4%bd%8d","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=189280","title":{"rendered":"JACS\uff1aRh1\/MoS2\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u7c7b\u9176\u56ca\u72b6\u6d3b\u6027\u4f4d\u70b9\u7528\u4e8e\u5df4\u8c46\u919b\u9009\u62e9\u6027\u52a0\u6c22"},"content":{"rendered":"

\u3010\u5f15\u8a00\u3011<\/b><\/strong><\/p>\n

\u4e0d\u9971\u548c\u919b\uff08\u4f8b\u5982\u5df4\u8c46\u919b\uff09\u7684\u9009\u62e9\u6027\u52a0\u6c22\u6210\u4e0d\u9971\u548c\u9187\u662f\u4e00\u7cfb\u5217\u91cd\u8981\u7684\u5de5\u4e1a\u53cd\u5e94\uff0c\u7528\u4e8e\u751f\u4ea7\u533b\u836f\u3001\u519c\u5316\u548c\u82b3\u9999\u5316\u5408\u7269\u7684\u4e2d\u95f4\u4f53\u3002\u7136\u800c\uff0c\u7531\u4e8eC\uff1dC\u952e\u7684\u52a0\u6c22\u6bd4C\uff1dO\u952e\u7684\u52a0\u6c22\u5bb9\u6613\u5f97\u591a\uff0c\u56e0\u6b64\u5b9e\u73b0\u8fd9\u79cd\u9ad8\u9009\u62e9\u6027\u548c\u7406\u60f3\u7684\u53cd\u5e94\u662f\u4e00\u9879\u8270\u5de8\u7684\u4efb\u52a1\u3002\u5747\u76f8\u50ac\u5316\u5242\u901a\u8fc7\u4ea7\u751f\u79bb\u5b50\u6c22\u6765\u6fc0\u6d3b\u6781\u5316\u7684\u53cc\u952e\uff08\u5982\u7fb0\u57fa\uff09\uff0c\u5bf9\u8fd9\u7c7b\u53cd\u5e94\u662f\u6709\u6548\u7684\u3002\u4f46\u8fd9\u4e9b\u5747\u76f8\u50ac\u5316\u5242\u88ab\u8ba4\u4e3a\u5bf9\u73af\u5883\u4e0d\u53cb\u597d\uff0c\u96be\u4ee5\u4e0e\u4ea7\u7269\u5206\u79bb\u3002\u56e0\u6b64\uff0c\u4ece\u4fc3\u8fdb\u5242\u3001\u53cc\u91d1\u5c5e\u50ac\u5316\u5242\u3001\u8fd8\u539f\u6027\u6c27\u5316\u7269\u3001\u91d1\u5c5e\u6709\u673a\u9aa8\u67b6\u5185\u914d\u4f4d\u4e0d\u9971\u548c\u91d1\u5c5e\u8282\u70b9\u7b49\u65b9\u5411\u5f00\u5c55\u591a\u76f8\u50ac\u5316\u5242\u7684\u7814\u7a76\uff0c\u4ee5\u514b\u670d\u70ed\u529b\u5b66\u7ea6\u675f\uff0c\u5b9e\u73b0\u9ad8\u9009\u62e9\u6027\u4e3a\u76ee\u6807\u3002\u5c06\u4e0d\u9971\u548c\u919b\u9009\u62e9\u6027\u52a0\u6c22\u4e3a\u4e0d\u9971\u548c\u9187\uff0c\u8981\u5b9e\u73b0100\uff05\u9009\u62e9\u6027\u4ecd\u7136\u662f\u4e00\u9879\u8270\u5de8\u7684\u4efb\u52a1\u3002\u9176\u662f\u4e00\u79cd\u9ad8\u9009\u62e9\u6027\u3001\u9ad8\u6d3b\u6027\u7684\u50ac\u5316\u5242\uff0c\u80fd\u9009\u62e9\u5355\u4e00\u7684\u5e95\u7269\u3002\u9176\u6d3b\u6027\u4f4d\u70b9\u7684\u7c7b\u9176\u56ca\u72b6\u7ed3\u6784\u5177\u6709\u72ec\u7279\u7684\u7a7a\u95f4\u6548\u5e94\uff0c\u53ef\u4ee5\u6709\u6548\u5730\u7b5b\u9009\u5206\u5b50\u5316\u5408\u7269\uff0c\u786e\u5b9a\u76ee\u6807\u5438\u9644\u4f4d\u70b9\u7684\u7279\u5b9a\u6784\u578b\uff0c\u4fc3\u8fdb\u4f4e\u80fd\u8dc3\u8fc1\u6001\u7684\u5f62\u6210\uff0c\u9650\u5236\u6784\u578b\u6784\u8c61\u4ea7\u751f\u5355\u4e00\u7684\u7406\u60f3\u4ea7\u7269\u3002\u9176\u7684\u9ad8\u9009\u62e9\u6027\u4e0d\u4ec5\u662f\u7531\u4e8e\u5176\u660e\u786e\u7684\u6d3b\u6027\u4f4d\u70b9\uff0c\u800c\u4e14\u8fd8\u7531\u4e8e\u5176\u7cbe\u786e\u63a7\u5236\u7684\u5438\u9644\u7ed3\u6784\u3002\u6700\u8fd1\u53d1\u5c55\u7684\u5355\u539f\u5b50\u50ac\u5316\u5242\uff08SACs\uff09\u5177\u6709\u5747\u5300\u7684\u5355\u6d3b\u6027\u4f4d\u70b9\uff0c\u6709\u5229\u4e8e\u9009\u62e9\u6027\u53cd\u5e94\u3002\u5728\u6d3b\u6027\u5355\u91d1\u5c5e\u4e2d\u5fc3\u5468\u56f4\u6784\u5efa\u7a7a\u95f4\u4f4d\u963b\u7684\u6d3b\u6027\u4f4d\u70b9\uff0c\u53ef\u4ee5\u8fdb\u4e00\u6b65\u63d0\u9ad8\u76ee\u6807\u53cd\u5e94\u5bf9\u7406\u60f3\u4ea7\u7269\u7684\u9009\u62e9\u6027\u3002<\/p>\n

\u3010\u6210\u679c\u7b80\u4ecb\u3011<\/b><\/strong><\/p>\n

\u8fd1\u65e5\uff0c\u5728\u7f8e\u56fd<\/b><\/strong>\u4e9a\u5229\u6851\u90a3\u5dde\u7acb\u5927\u5b66Jingyue Liu\u6559\u6388<\/b><\/strong>\u548c\u5fb7\u514b\u8428\u65af\u5927\u5b66\u8fbe\u62c9\u65af<\/b><\/strong>\u5206\u6821<\/b><\/strong>Kyeongjae Cho\u6559\u6388\u56e2\u961f\uff08\u5171\u540c\u901a\u8baf\u4f5c\u8005\uff09<\/b><\/strong>\u5e26\u9886\u4e0b\uff0cDr.\u00a0Yang Lou (now at\u6c5f\u5357\u5927\u5b66)\u00a0and Dr. Yongping Zheng (now at\u4e2d\u79d1\u9662\u6df1\u5733\u5148\u8fdb\u6280\u672f\u7814\u7a76\u6240) \u62a5\u9053\u4e86\u951a\u5b9a\u57282D MoS2<\/sub>\u7247\u8fb9\u7f18\u4e0a\u7684\u5355\u4e2aRh\u539f\u5b50\u53ef\u4ee5\u901a\u8fc7\u7c7b\u9176\u56ca\u72b6\u6d3b\u6027\u4f4d\u70b9\u7684\u7a7a\u95f4\u9650\u5236\u6548\u5e94\uff0c\u5c06\u5df4\u8c46\u919b\u6709\u6548\u5730\u8f6c\u5316\u4e3a\u5df4\u8c46\u9187\uff0c\u5e76\u5177\u6709100\uff05\u7684\u9009\u62e9\u6027\u3002\u8868\u5f81\u7ed3\u679c\u8868\u660e\uff0c\u5408\u6210\u7684Rh1<\/sub>\/MoS2<\/sub>\u5355\u539f\u5b50\u50ac\u5316\u5242\uff08SACs\uff09\u5177\u6709\u72ec\u7279\u7684\u51e0\u4f55\u548c\u7535\u5b50\u6784\u578b\uff0c\u901a\u8fc7\u7a7a\u95f4\u6548\u5e94\u9650\u5236\u4e86\u53cd\u5e94\u7269\u5206\u5b50\u7684\u5438\u9644\u6a21\u5f0f\u3002DFT\u8ba1\u7b97\u8868\u660e\uff0cMoS2<\/sub>\u7247\u7ec8\u6b62\u4e8e\u6c27\u5316\u7684Mo\u8fb9\u7f18\uff0cRh1<\/sub>\u7a33\u5b9a\u5730\u951a\u5b9a\u5728Mo\u9633\u79bb\u5b50\u7a7a\u4f4d\u5904\uff0c\u4ece\u800c\u53ef\u4ee5\u5bb9\u6613\u5730\u5c06H2<\/sub>\u89e3\u79bb\u4e3aH\u539f\u5b50\u3002\u79bb\u89e3\u7684H\u539f\u5b50\u6ea2\u51fa\u4e0e\u8fb9\u7f18O\u539f\u5b50\u53cd\u5e94\u5f62\u6210OH\u7269\u79cd\uff0c\u5f62\u6210HO-Mo-Rh1<\/sub>-Mo-OH\u6784\u578b\uff0c\u7c7b\u4f3c\u4e8e\u7c7b\u9176\u56ca\u72b6\u6d3b\u6027\u4f4d\uff0c\u8fd9\u7531\u4e8e\u7a7a\u95f4\u6548\u5e94\u800c\u9650\u5236\u4e86\u5df4\u8c46\u919b\u7684\u5438\u9644\u6a21\u5f0f\u3002\u8fd9\u79cd\u7279\u5b9a\u7684\u5438\u9644\u6784\u578b\u4ea7\u751f100\uff05\u7684\u9009\u62e9\u6027\u3002\u5229\u7528\u5355\u4e2a\u91d1\u5c5e\u539f\u5b50\u548c2D\u7eb3\u7c73\u7247\u6784\u9020\u7c7b\u9176\u56ca\u72b6\u6d3b\u6027\u4e2d\u5fc3\u7684\u7b56\u7565\u4e3a\u8bbe\u8ba1\u7528\u4e8e\u7279\u5b9a\u50ac\u5316\u8f6c\u5316\u7684\u9ad8\u9009\u62e9\u6027SACs\u5f00\u8f9f\u4e86\u65b0\u9014\u5f84\u3002\u76f8\u5173\u6210\u679c\u4ee5\u9898\u4e3a\u201c<\/b><\/strong>Pocket-like active site of Rh<\/b><\/strong>1<\/b><\/sub><\/strong>\/MoS<\/b><\/strong>2<\/b><\/sub><\/strong>\u00a0single-atom catalyst for selective crotonaldehyde hydrogenation<\/b><\/strong>\u201d<\/b><\/strong>\u53d1\u8868\u5728\u4e86J. Am. Chem. Soc.<\/b><\/strong>\u4e0a\u3002<\/p>\n

\u3010\u56fe\u6587\u5bfc\u8bfb\u3011<\/b><\/strong><\/p>\n

\u56fe1<\/b><\/strong>\u00a0<\/b><\/strong>Rh<\/b><\/strong>1<\/b><\/sub><\/strong>\/<\/b><\/strong>MoS<\/b><\/strong>2<\/b><\/sub><\/strong>\u00a0SAC\u7684HAADF<\/b><\/strong>–<\/b><\/strong>STEM\u56fe\u50cf<\/b><\/strong>\"\"<\/p>\n

\uff08a\uff09Rh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u7684\u4ee3\u8868\u6027\u539f\u5b50\u5206\u8fa8\u7387HAADF-STEM\u56fe\u50cf\u3002\u56fe\u4e2d\u7684\u767d\u70b9\u4ee3\u8868\u5355\u4e2aRh1<\/sub>\u539f\u5b50\u3002\u4e3a\u4e86\u6e05\u695a\u8d77\u89c1\uff0c\u5c3d\u7ba1\u56fe\u50cf\u4e2d\u542b\u6709\u66f4\u591a\u7684MoS2<\/sub>\u8fb9\u7f18\u951a\u5b9a\u7684Rh1<\/sub>\u539f\u5b50\uff0c\u4f46\u53ea\u6709\u5c11\u6570\u51e0\u4e2a\u5b64\u7acb\u7684Rh1<\/sub>\u539f\u5b50\u7528\u9ec4\u8272\u7bad\u5934\u6807\u8bb0\u3002<\/p>\n

\uff08b\uff09\u4e09\u6b21\u9009\u62e9\u6027\u52a0\u6c22\u53cd\u5e94\u540e\u7684HAADF-STEM\u56fe\u3002<\/p>\n

\uff08c\uff09Rh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u3001\u7eb3\u7c73Rh\/MoS2<\/sub>\u548cRh\u7b94\u7684Rh K-edge EXAFS\u5149\u8c31\u3002<\/p>\n

\uff08d\uff09DFT\u8ba1\u7b97\u4e86Rh1<\/sub>\u6d3b\u6027\u4f4d\u70b9\u7684\u7a33\u5b9aRh1<\/sub>-S4<\/sub>\u6784\u578b\u3002<\/p>\n

\u00a0<\/b><\/strong>\u56fe2<\/b><\/strong>\u00a0<\/b><\/strong>Rh<\/b><\/strong>1<\/b><\/sub><\/strong>\/<\/b><\/strong>MoS<\/b><\/strong>2<\/b><\/sub><\/strong>\u00a0SAC\u9009\u62e9\u6027\u52a0\u6c22\u7684\u50ac\u5316\u6027\u80fd<\/b><\/strong>\"\"<\/p>\n

\uff08a,b\uff09MoS2<\/sub>\u3001\u7eb3\u7c73Rh\/MoS2<\/sub>\u548cRh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u7684\u9009\u62e9\u6027\u5df4\u8c46\u919b\u52a0\u6c22\u5236\u5df4\u8c46\u9187\u7684\u50ac\u5316\u6027\u80fd\uff1a\u8f6c\u6362\u6570\uff08a\uff09\u548c\u9009\u62e9\u6027\uff08b\uff09\u3002\u00a0<\/p>\n

\uff08c\uff09Rh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u7684\u8f6c\u5316\u7387\u548c\u9009\u62e9\u6027\u3002\u00a0<\/p>\n

\uff08d\uff09Rh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u7684\u7a33\u5b9a\u6027\u548c\u7a33\u5b9a\u6027\u3002<\/p>\n

\u53cd\u5e94\u6761\u4ef6\uff1a20.5 L\u5df4\u8c46\u919b\u57288 ml\u4e59\u9187\u6eb6\u6db2\u548c5 bar H2<\/sub>\u4e0b\uff0c\u572880\u2103\u4e0b\u53cd\u5e942.5-3.5\u5c0f\u65f6\uff0c\u4e0d\u540c\u50ac\u5316\u5242\u7684\u91cd\u91cf\u4ece20 mg\u5230150 mg\u3002<\/p>\n

\u56fe3<\/b><\/strong>\u00a0<\/b><\/strong>Rh<\/b><\/strong>1<\/b><\/sub><\/strong>\/<\/b><\/strong>MoS<\/b><\/strong>2<\/b><\/sub><\/strong>\u00a0SAC<\/b><\/strong>\u50ac\u5316\u5242\u7684\u539f\u4f4dCO-DRIFTS<\/b><\/strong>\"\"<\/p>\n

\uff08a\uff09MoS2<\/sub>\u3001\u7eb3\u7c73Rh\/MoS2<\/sub>\u548cRh1<\/sub>\/MoS2<\/sub>\u00a0SAC\u50ac\u5316\u5242\u7684\u539f\u4f4dCO-DRIFTS\u3002<\/p>\n

\uff08b\uff09DFT\u7406\u8bba\u8ba1\u7b97\uff1a\u5728MoS2<\/sub>\u8fb9\u7f18\u951a\u5b9a\u7684\u5355\u4e2aRh1<\/sub>\u539f\u5b50\u4e0a\u6a21\u62df\u7684CO\u5438\u9644\u6a21\u5f0f\u3002CO\u5438\u9644\u5b9e\u9a8c\u572830\u2103\u4e0b\u8fdb\u884c\u3002<\/p>\n

\u56fe<\/b><\/strong>4 <\/b><\/strong>\u5355\u4e2aRh<\/b><\/strong>1<\/b><\/sub><\/strong>\u539f\u5b50\u4e0a\u9009\u62e9\u6027\u5df4\u8c46\u919b<\/b><\/strong>\u52a0\u6c22<\/b><\/strong>\u7684<\/b><\/strong>DFT\u8ba1\u7b97<\/b><\/strong>\"\"<\/p>\n

DFT\u8ba1\u7b97\u5728\u5355\u4e2aRh1<\/sub>\u539f\u5b50\u4e0a\u9009\u62e9\u6027\u5df4\u8c46\u919b\u52a0\u6c22\u7684\u53cd\u5e94\u5468\u671f\uff0c\u8be5\u5355\u4e2aRh1<\/sub>\u539f\u5b50\u951a\u5b9a\u5728MoS2<\/sub>\u7684Mo\u8fb9\u7f18\u7a7a\u4f4d\uff08VMo<\/sub>\uff09\u4f4d\u70b9\u4e0a\uff0c\u5f62\u6210HO-Mo-Rh1<\/sub>-Mo-OH\u53e3\u888b\u72b6\u6d3b\u6027\u4f4d\u70b9\u3002Mo\u3001Rh\u3001O\u3001H\u3001C\u3001S\u5206\u522b\u4e3a\u9752\u8272\u3001\u6d45\u7070\u8272\u3001\u7ea2\u8272\u3001\u6d45\u7c89\u7ea2\u8272\u3001\u68d5\u8272\u3001\u9ec4\u8272\u3002<\/p>\n

\u3010\u5c0f\u7ed3<\/b><\/strong>\u3011<\/p>\n

\u603b\u4e4b\uff0c\u56e2\u961f\u8bbe\u8ba1\u548c\u5236\u5907\u4e86\u5177\u6709\u7c7b\u9176\u56ca\u72b6\u6d3b\u6027\u4f4d\u70b9\u7684Rh1<\/sub>\/MoS2<\/sub>\u00a0SACs\uff0c\u5df4\u8c46\u919b\u6c22\u5316\u4e3a\u5df4\u8c46\u9187\u7684\u9009\u62e9\u6027\u4e3a100\uff05\u3002\u5b9e\u9a8c\u7ed3\u679c\u548cDFT\u8ba1\u7b97\u5747\u8868\u660e\uff0c\u7531HO-Mo-Rh1<\/sub>-Mo-OH\u4f5c\u4e3a\u6d3b\u6027\u4f4d\u70b9\u7ec4\u6210\u7684\u7c7b\u9176\u56ca\u72b6\u6784\u578b\uff0c\u5176\u51e0\u4f55\u6784\u578b\u4ee5\u53ca\u7535\u5b50\u7ed3\u6784\u5bf9\u53cd\u5e94\u9009\u62e9\u6027\u6709\u663e\u8457\u7684\u5f71\u54cd\u3002\u9ad8\u9009\u62e9\u6027\u6c22\u5316\u6d3b\u6027\u53ef\u80fd\u6e90\u4e8e\u4fee\u9970\u7684MoS2<\/sub>\u7eb3\u7c73\u7247\u8fb9\u7f18\u7684OH\u57fa\u56e2\u3002\u8fdb\u4e00\u6b65\u6539\u8fdb\u4f18\u5316\u53e3\u888b\u72b6\u6d3b\u6027\u4f4d\u70b9\u548c\u53cd\u5e94\u6761\u4ef6\u53ef\u80fd\u4f1a\u8fdb\u4e00\u6b65\u663e\u8457\u63d0\u9ad8\u53cd\u5e94\u6d3b\u6027\u3002\u5229\u7528\u5355\u91d1\u5c5e\u539f\u5b50\u548c2D\u7eb3\u7c73\u7ed3\u6784\u7684\u72ec\u7279\u6027\u8d28\u6784\u5efa\u53e3\u888b\u72b6\u6d3b\u6027\u4f4d\u70b9\u7684\u7b56\u7565\u6709\u671b\u4e3a\u5f00\u53d1\u591a\u79cd\u6db2\u76f8\u548c\u6c14\u76f8\u9009\u62e9\u6027\u52a0\u6c22\/\u6c27\u5316\u53cd\u5e94\u7684\u9ad8\u9009\u62e9\u6027\u50ac\u5316\u5242\u5f00\u8f9f\u65b0\u9014\u5f84\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1a<\/b><\/strong>Pocket-like active site of Rh<\/u>1<\/sub><\/u>\/MoS<\/u>2<\/sub><\/u>\u00a0single-atom catalyst for selective crotonaldehyde hydrogenation<\/u><\/a>\uff08J. Am. Chem. Soc., 2019, DOI:10.1021\/jacs.9b06628\uff09<\/p>\n

\u672c\u6587\u7531\u6728\u6587\u97ec<\/b><\/strong>\u7ffb\u8bd1\uff0c\u6750\u6599\u725b\u6574\u7406\u7f16\u8f91\u3002<\/p>\n

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