{"id":154771,"date":"2018-09-28T06:30:14","date_gmt":"2018-09-27T22:30:14","guid":{"rendered":"\/\/m.iemloyee.com\/?p=154771"},"modified":"2018-09-27T20:03:55","modified_gmt":"2018-09-27T12:03:55","slug":"j-am-chem-soc-%e5%85%89%e6%95%8f%e9%87%91%e5%b1%9e%e6%9c%89%e6%9c%ba%e5%8d%95%e5%b1%82%e6%9d%90%e6%96%99%e5%ba%94%e7%94%a8%e4%ba%8e%e6%97%a5%e5%85%89%e9%a9%b1%e5%8a%a8%e7%9a%84","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=154771","title":{"rendered":"J. Am. Chem. Soc.: \u5149\u654f\u91d1\u5c5e\u6709\u673a\u5355\u5c42\u6750\u6599\u5e94\u7528\u4e8e\u65e5\u5149\u9a71\u52a8\u7684\u9ad8\u6548CO2\u8fd8\u539f"},"content":{"rendered":"
\u3010\u5f15\u8a00\u3011<\/strong><\/p>\n \n \u91d1\u5c5e\u6709\u673a\u6846\u67b6(MOFs)\u4e3a\u7814\u7a76\u5305\u62ec\u5236\u6c22\u3001CO2<\/sub>\u8fd8\u539f\u3001\u4ea7\u6c27\u5728\u5185\u7684\u4eba\u5de5\u5149\u5408\u4f5c\u7528\u63d0\u4f9b\u4e86\u4e00\u79cd\u591a\u529f\u80fd\u6750\u6599\u5e73\u53f0\u3002MOFs\u7684\u7ed3\u6784\u89c4\u5f8b\u6027\u548c\u5408\u6210\u53ef\u8c03\u6027\u53ef\u5206\u7ea7\u6574\u5408\u591a\u4e2a\u529f\u80fd\u6a21\u5757(\u5305\u62ec\u5149\u654f\u5242(PS)\u548c\u50ac\u5316\u4e2d\u5fc3)\uff0c\u4ee5\u4fc3\u8fdb\u5149\u53cd\u5e94\u4e2d\u7684\u591a\u7535\u5b50\u6216\u81ea\u7531\u57fa\u8f6c\u79fb\u3002\u7136\u800c\uff0c\u7531\u4e8e\u5927\u591a\u6570\u5149\u654f\u5242\u7684\u672c\u5f81\u9ad8\u5438\u6536\u7387\uff0c\u53ea\u6709\u8868\u9762\u7684MOF\u5c42\u80fd\u591f\u53c2\u4e0e\u5149\u53cd\u5e94\uff0c\u800c\u4e14MOF\u9897\u7c92\u7684\u5149\u6563\u5c04\u4f1a\u964d\u4f4e\u5149\u5b50\u5229\u7528\u7387\u3002\u6b64\u5916\uff0c\u81ea\u7531\u57fa\u548c\u5176\u4ed6\u80fd\u91cf\u4e2d\u95f4\u4f53\u901a\u8fc7MOF\u901a\u9053\u65f6\u7684\u9650\u5236\u6027\u6269\u6563\u4e5f\u51cf\u5f31\u4e86MOF\u7684\u5149\u50ac\u5316\u6548\u7387\u3002\u56e0\u6b64\uff0c\u5c06MOF\u7684\u4e00\u4e2a\u7ef4\u5ea6\u5c3a\u5bf8\u51cf\u5c0f\u5230\u5355\u5c42(<2 nm)\u540e\uff0c\u6240\u5f97\u7684\u91d1\u5c5e\u6709\u673a\u5355\u5c42(MOL)\u4f5c\u4e3a\u4e00\u7c7b\u65b0\u578b\u53ef\u529f\u80fd\u53162D\u6750\u6599\u5728\u4eba\u5de5\u5149\u5408\u4f5c\u7528\u9886\u57df\u5177\u6709\u5e7f\u9614\u7684\u524d\u666f\u3002\u5728\u8bb8\u591a\u7528\u4e8eCO2\u8fd8\u539f\u7684\u5149\u50ac\u5316\u4f53\u7cfb\u4e2d\uff0c\u4f5c\u4e3a\u5149\u654f\u5242\u7684[Ru(bpy)3<\/sub>]2+<\/sup>(bpy = 2,2′-\u8054\u5421\u5576)\u548c\u4f5c\u4e3aCO2<\/sub>\u8fd8\u539f\u50ac\u5316\u5242\u7684ReI<\/sup>(bpy)(CO)3<\/sub>Cl\u7684\u7ec4\u5408\u7531\u4e8e\u5176\u80fd\u591f\u4ee5\u9ad8\u9009\u62e9\u6027\u548c\u9ad8\u6548\u7387\u4ea7\u751fCO\uff0c\u5f97\u5230\u4e86\u5e7f\u6cdb\u7684\u7814\u7a76\u3002<\/p>\n \u3010\u6210\u679c\u7b80\u4ecb\u3011<\/strong><\/p>\n \n \u8fd1\u65e5\uff0c\u7f8e\u56fd\u829d\u52a0\u54e5\u5927\u5b66\u548c\u53a6\u95e8\u5927\u5b66\u7684\u6797\u6587\u658c\u6559\u6388(\u901a\u8baf\u4f5c\u8005)\u7b49<\/strong>\u8bbe\u8ba1\u4e86\u57fa\u4e8eHf12<\/sub>\u4e8c\u7ea7\u6784\u5efa\u5355\u5143(SBU)\u548c[Ru(bpy)3<\/sub>]2+<\/sup>(bpy = 2,2′-\u8054\u5421\u5576)\u884d\u751f\u7684\u4e8c\u7fa7\u9178\u914d\u4f53\u7684\u65b0\u578b\u5149\u654fMOL\u2014\u2014Hf12<\/sub>-Ru\uff0c\u5e76\u5728J. Am. Chem. Soc.<\/strong>\u4e0a\u53d1\u8868\u4e86\u9898\u4e3a\u201cPhotosensitizing Metal-Organic Layers for Efficient Sunlight-Driven Carbon Dioxide Reduction<\/strong>\u201d\u7684\u7814\u7a76\u8bba\u6587\u3002\u5229\u7528M(bpy)(CO)3<\/sub>X(M = Re\u548cX = Cl\u6216M = Mn\u548cX = Br)\u884d\u751f\u7684\u5355\u7fa7\u9178\u5206\u5b50\u901a\u8fc7\u7fa7\u9178\u4ea4\u6362\u53cd\u5e94\u7f6e\u6362\u6389Hf12<\/sub>-Ru\u7684\u4e8c\u7ea7\u6784\u5efa\u5355\u5143\u8868\u9762\u5c01\u7aef\u7684\u4e09\u6c1f\u4e59\u9178\u57fa\u56e2\u540e\uff0c\u6240\u5f97\u7684Hf12<\/sub>-Ru-Re \u548cHf12<\/sub>-Ru-Mn MOL\u540c\u65f6\u5177\u6709[Ru(bpy)3<\/sub>]2+<\/sup>\u5149\u654f\u5242\u548cM(bpy)(CO)3<\/sub>X\u50ac\u5316\u5242\uff0c\u53ef\u6709\u6548\u5730\u5149\u50ac\u5316\u8fd8\u539fCO2<\/sub>\u3002MOL\u9aa8\u67b6\u4e0e\u5c01\u7aef\u914d\u4f53\u8f83\u77ed\u7684\u8ddd\u79bb(1-2nm)\u4fc3\u8fdb\u4e86\u4ece\u5149\u6fc0\u53d1\u7684[Ru(bpy)3<\/sub>]2+<\/sup>*\u5230MI<\/sup>(bpy)(CO)3<\/sub>X(M = Re, Mn)\u50ac\u5316\u4e2d\u5fc3\u7684\u591a\u7535\u5b50\u8f6c\u79fb\uff0c\u5728\u4eba\u5de5\u53ef\u89c1\u5149\u4e0bCO2<\/sub>\u8fd8\u539f\u8f6c\u5316\u6570\u4e3a8613\uff0c\u9633\u5149\u4e0b\u4e3a670\u3002\u56e0\u6b64\uff0cMOL\u4f5c\u4e3a\u4e00\u7c7b\u7528\u4e8e\u7814\u7a76\u4eba\u5de5\u5149\u5408\u4f5c\u7528\u7684\u7ec4\u88c5\u591a\u529f\u80fd\u6750\u6599\u5177\u6709\u5e7f\u9614\u7684\u7814\u7a76\u524d\u666f\u3002<\/p>\n \u3010\u56fe\u6587\u7b80\u4ecb\u3011<\/strong> Hf12<\/sub>-Ru\u901a\u8fc7\u5355\u7fa7\u9178\u4ea4\u6362\u5408\u6210Hf12<\/sub>-Ru-M (M = Re\u6216Mn)\u7684\u793a\u610f\u56fe\u53ca\u5176\u65e5\u5149\u9a71\u52a8CO2<\/sub>\u8fd8\u539f\u3002<\/p>\n \u56fe2 Hf12<\/sub>-Ru\u7684\u7ed3\u6784\u3001\u5f62\u8c8c\u8868\u5f81<\/strong><\/p>\n a) Hf12<\/sub>-Ru\u7684TEM\u56fe\u50cf\uff1b \u56fe3 Hf12<\/sub>-Ru-Re\u7684\u5f62\u8c8c\u3001\u7ed3\u6784\u8868\u5f81<\/strong><\/p>\n a) \u6d88\u89e3\u540eHf12<\/sub>-Ru-MBA\u7684NMR\u5149\u8c31\uff0c\u9ec4\u8272\u548c\u7eff\u8272\u661f\u53f7\u5206\u522b\u5f52\u5c5e\u4e8eL-Ru\u914d\u4f53\u548cMBA\u914d\u4f53\uff1b \u56fe4 \u50ac\u5316\u5242\u7684\u5149\u8fd8\u539fCO2<\/sub>\u6027\u80fd<\/strong><\/p>\n a) Hf12<\/sub>-Ru-Re\u7684CO\u4ea7\u751f\u8f6c\u5316\u6570\u968f\u65f6\u95f4\u7684\u53d8\u5316\uff1b \u56fe5 Hf12<\/sub>-Ru-Re\u7684\u65e5\u5149\u9a71\u52a8CO2<\/sub>\u8fd8\u539f\u6027\u80fd<\/strong><\/p>\n 6 h\u5185Hf12<\/sub>-Ru-Re\u7684\u65e5\u5149\u9a71\u52a8CO2<\/sub>\u8fd8\u539fTONs\u3002<\/p>\n \u3010\u5c0f\u7ed3\u3011<\/strong>
\n \u56fe1 Hf12<\/sub>-Ru-M (M = Re\u6216Mn)\u5408\u6210\u8fc7\u7a0b\u793a\u610f\u56fe<\/strong><\/p>\n<\/p>\n
<\/p>\n
\n b) Hf12<\/sub>-Ru\u7684HRTEM\u56fe\u50cf\uff1b
\n c) Hf12<\/sub> MOLs\u7684PXRD\u56fe\u8c31\uff1b
\n d) Hf12<\/sub>-Ru\u7684AFM\u56fe\u50cf\uff1b
\n e) Hf12<\/sub>-Ru\u7684\u9ad8\u5ea6\u66f2\u7ebf\uff1b
\n f) Hf12<\/sub>\u7c07\u4ee5TFA\u57fa\u56e2\u5c01\u7aef\u7684\u793a\u610f\u56fe\u3002<\/p>\n<\/p>\n
\n b) Hf12<\/sub>-Ru-Re\u7684TEM\u56fe\u50cf\uff1b
\n c) Hf12<\/sub>-Ru-Re\u7684EXAFS\u62df\u5408\uff1b
\n d) Hf12<\/sub>-Ru-Re\u7684AFM\u56fe\u50cf\uff1b
\n e) Hf12<\/sub>-Ru-Re\u7684\u9ad8\u5ea6\u66f2\u7ebf\u3002<\/p>\n<\/p>\n
\n b) Hf12<\/sub>-Ru-Mn\u7684CO\u4ea7\u751f\u8f6c\u5316\u6570\u968f\u65f6\u95f4\u7684\u53d8\u5316\uff1b
\n c) Hf12<\/sub>-Ru\u3001Hf12<\/sub>-Ru-Re\u548cHf12<\/sub>-Ru-Mn\u5149\u50ac\u5316\u540e\u7684PXRD\u56fe\u8c31\uff1b
\n d) Hf12<\/sub>-Ru-Re\u8fde\u7eed5\u6b21\u5faa\u73af\u7684CO\u4ea7\u751f\u8f6c\u5316\u6570\u3002<\/p>\n<\/p>\n
\n \u7efc\u4e0a\u6240\u8ff0\uff0c\u7814\u7a76\u4eba\u5458\u9996\u6b21\u5408\u6210\u4e86\u57fa\u4e8e\u6613\u4e8e\u5b98\u80fd\u5316\u7684\u7ebf\u6027\u4e8c\u7fa7\u9178\u914d\u4f53\u7684MOL\u3002 \u4e4b\u540e\u5229\u7528\u7fa7\u9178\u4ea4\u6362\u53cd\u5e94\u5c06\u5149\u654fHf12<\/sub>-Ru MOL\u4e0eM(bpy)(CO)3<\/sub>X(M = Re\u6216Mn)\u57fa\u56e2\u8fdb\u884c\u540e\u5408\u6210\u5b98\u80fd\u5316\u53cd\u5e94\uff0c\u5f97\u5230\u4e24\u79cd\u540c\u65f6\u5177\u6709[Ru(bpy)3<\/sub>]2+<\/sup>\u5149\u654f\u5242\u548cM(bpy)(CO)3<\/sub>X\u50ac\u5316\u5242\u7684MOLs\u2014\u2014Hf12<\/sub>-Ru-Re\u548cHf12<\/sub>-Ru-Mn\uff0c\u5176\u53ef\u7528\u4e8e\u9ad8\u6548\u5149\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u3002\u4f5c\u8005\u53d1\u73b0\uff0c\u5149\u654fMOL\u6846\u67b6\u4e0e\u5c01\u7aefCO2<\/sub>\u8fd8\u539f\u50ac\u5316\u5242\u8ddd\u79bb\u7684\u7f29\u77ed\u6781\u5927\u5730\u4fc3\u8fdb\u4e86\u4ece\u5149\u8fd8\u539f[Ru(bpy)3<\/sub>]2+<\/sup>*\u5230MI<\/sup>(bpy)(CO)3<\/sub>X(M = Re, Mn)\u50ac\u5316\u4e2d\u5fc3\u7684\u591a\u7535\u5b50\u8f6c\u79fb\u3002 Hf12<\/sub>-Ru-Re\u4f53\u7cfb\u5728\u4eba\u5de5\u53ef\u89c1\u5149\u4e0b\u7684CO2<\/sub>\u8fd8\u539f\u8f6c\u5316\u6570\u4e3a8613\uff0c\u5728\u9633\u5149\u4e0b\u4e3a670\u3002 \u56e0\u6b64\uff0c\u8be5\u5de5\u4f5c\u53ef\u4e3a\u592a\u9633\u80fd\u80fd\u6e90\u76f8\u5173\u7684\u591a\u529f\u80fdMOL\u7684\u8bbe\u8ba1\u548c\u6784\u7b51\u63d0\u4f9b\u6307\u5bfc\u3002<\/p>\n