{"id":231322,"date":"2021-12-30T06:08:36","date_gmt":"2021-12-29T22:08:36","guid":{"rendered":"\/\/m.iemloyee.com\/?p=231322"},"modified":"2021-12-29T20:08:49","modified_gmt":"2021-12-29T12:08:49","slug":"%e6%b1%9f%e6%b5%b7%e9%be%99%e5%9b%a2%e9%98%9f-angew-%ef%bc%9apd3cuuio-66%e5%85%89%e8%be%85%e5%8a%a9%e5%82%ac%e5%8c%96co2%e5%8a%a0%e6%b0%a2","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=231322","title":{"rendered":"\u6c5f\u6d77\u9f99\u56e2\u961f Angew.\uff1aPd3Cu@UiO-66\u5149\u8f85\u52a9\u50ac\u5316CO2\u52a0\u6c22"},"content":{"rendered":"
\u3010\u80cc\u666f\u4ecb\u7ecd\u3011<\/strong><\/p>\n \u968f\u7740\u5de5\u4e1a\u5316\u8fdb\u7a0b\u7684\u5feb\u901f\u63a8\u8fdb\uff0c\u5927\u6c14\u4e2d\u4e8c\u6c27\u5316\u78b3\uff08CO2<\/sub>\uff09\u6d53\u5ea6\u4e0d\u65ad\u589e\u52a0\uff0c\u4ece\u800c\u5f15\u53d1\u4e86\u5168\u7403\u53d8\u6696\u7b49\u5371\u673a\u3002\u5728\u4f17\u591a\u7684CO2<\/sub>\u6355\u96c6\u4e0e\u8f6c\u5316\u6280\u672f\u4e2d\uff0c\u5c06CO2<\/sub>\u52a0\u6c22\u8f6c\u5316\u4e3a\u7532\u9178\uff08HCOOH\uff09\u3001\u7532\u9187\uff08CH3<\/sub>OH\uff09\u548c\u7532\u70f7\uff08CH4<\/sub>\uff09\u7b49\u589e\u503c\u5316\u5b66\u54c1\u88ab\u8ba4\u4e3a\u662f\u884c\u4e4b\u6709\u6548\u7684\u7b56\u7565\u3002\u5176\u4e2d\uff0c\u7532\u9187\u662f\u8fde\u63a5\u4e0a\u6e38C1<\/sub>\u5c0f\u5206\u5b50\u4e0e\u4e0b\u6e38\u5927\u5b97\u5316\u5b66\u54c1\u548c\u71c3\u6599\u7684\u91cd\u8981\u5316\u5de5\u539f\u6599\u3002\u76ee\u524d\uff0c\u901a\u8fc7\u7535\u3001\u5149\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u5f97\u5230\u7532\u9187\u5f80\u5f80\u9762\u4e34\u6548\u7387\u4f4e\uff1b\u70ed\u50ac\u5316CO2<\/sub>\u5f80\u5f80\u9700\u8981\u9ad8\u6e29\u9ad8\u538b\uff0850-100 bar\u3001200-300 \u00b0C\uff09\u7684\u82db\u523b\u6761\u4ef6\uff0c\u800c\u5728\u9ad8\u6e29\u4e0b\u5f80\u5f80\u66f4\u5bb9\u6613\u53d1\u751f\u9006\u6c34\u7164\u6c14\u8f6c\u6362\uff08RWGS\uff09\u526f\u53cd\u5e94\uff0c\u4e0d\u5229\u4e8e\u9ad8\u9009\u62e9\u6027\u7684\u5236\u5907\u7532\u9187\u3002\u56e0\u6b64\uff0c\u5f00\u53d1\u4e00\u79cd\u80fd\u591f\u5728\u76f8\u5bf9\u4f4e\u6e29\u4e0b\u9ad8\u6548\uff0c\u9ad8\u9009\u62e9\u6027\u50ac\u5316CO2<\/sub>\u52a0\u6c22\u5236\u7532\u9187\u7684\u50ac\u5316\u5242\u81f3\u5173\u91cd\u8981\u3002\u91d1\u5c5e\u6709\u673a\u9aa8\u67b6\uff08MOFs\uff09\u662f\u4e00\u7c7b\u65b0\u578b\u7684\u6676\u6001\u591a\u5b54\u6750\u6599\uff0c\u5177\u6709\u7075\u6d3b\u7684\u7ed3\u6784\u53ef\u88c1\u526a\u6027\uff0c\u662f\u5236\u5907\u8fd9\u79cd\u591a\u529f\u80fd\u50ac\u5316\u5242\u7684\u7406\u60f3\u6750\u6599\u3002\u7136\u800c\uff0c\u57fa\u4e8eMOF\u57fa\u6750\u6599\u4e0a\u5f15\u5165\u592a\u9633\u80fd\u9a71\u52a8\u70ed\u50ac\u5316CO2<\/sub>\u52a0\u6c22\u5236\u7532\u9187\u7684\u7814\u7a76\u5c1a\u672a\u62a5\u9053\u3002 \u8fd1\u65e5\uff0c\u4e2d\u56fd\u79d1\u5b66\u6280\u672f\u5927\u5b66\u6c5f\u6d77\u9f99\u6559\u6388\uff08\u901a\u8baf\u4f5c\u8005\uff09\u7b49\u4eba<\/strong>\u62a5\u9053\u4e86\u5c06\u53cc\u91d1\u5c5ePd3<\/sub>Cu NPs\u5f15\u5165\u5230\u7ecf\u5178\u7684\u91d1\u5c5e\u6709\u673a\u9aa8\u67b6\u6750\u6599UiO-66\u4e2d\uff0c\u5f97\u5230Pd3<\/sub>Cu@UiO-66\u590d\u5408\u6750\u6599\uff0c\u5e76\u7528\u4e8e\u5149\u8f85\u52a9\u6761\u4ef6\u4e0b\u7684CO2<\/sub>\u52a0\u6c22\u53cd\u5e94\u3002\u7814\u7a76\u53d1\u73b0\uff0cZr-oxo\u7c07\u4e0a\u7684\u7f3a\u9677\u4f4d\u70b9\u80fd\u591f\u6355\u83b7\u548c\u6d3b\u5316CO2<\/sub>\u5206\u5b50\uff0cPd3<\/sub>Cu NPs\u53ef\u4ee5\u9ad8\u6548\u6d3b\u5316H2<\/sub>\u3002\u540c\u65f6\uff0cMOF\u914d\u4f53\u53ef\u4ee5\u6355\u83b7\u5149\u5b50\u5e76\u5149\u751f\u7535\u5b50\uff0c\u5149\u751f\u7535\u5b50\u901a\u8fc7LCCT\uff08\u914d\u4f53\u5230\u7c07\u7684\u7535\u8377\u8f6c\u79fb\uff09\u8fc7\u7a0b\u5c06\u5149\u751f\u7535\u5b50\u6ce8\u5165\u5230\u5438\u9644\u5728Zr-oxo\u7c07\u4e0a\u7684CO2<\/sub>\u7684\u53cd\u952e\u8f68\u9053\uff0c\u52a0\u901f\u4e86\u4e2d\u95f4\u7269\u79cdHCOO*\u7684\u751f\u6210\uff0c\u4ece\u800c\u663e\u8457\u964d\u4f4e\u4e86\u6574\u4e2a\u53cd\u5e94\u7684\u8868\u89c2\u6d3b\u5316\u80fd\u3002\u57fa\u4e8ePd3<\/sub>Cu@UiO-66\u4e8c\u6c27\u5316\u78b3\u52a0\u6c22\u50ac\u5316\u5242\u4e2d\u6210\u529f\u6784\u7b51\u4e86\u8fd1\u90bb\u7684CO2<\/sub>\u548cH2<\/sub>\u6d3b\u5316\u4f4d\u70b9\uff0c\u5728200 \u00b0C\u548c1.25 MPa\uff0cPd3<\/sub>Cu@UiO-66\u5728\u5149\u8f85\u52a9\u4e0b\u5b9e\u73b0\u4e86340 \u00b5mol g-1<\/sup> h-1<\/sup>\u7684\u7532\u9187\u4ea7\u7387\uff0c\u9ad8\u51fa\u9ed1\u6697\u6761\u4ef6\u4e0b\u50ac\u5316\u6027\u80fd\u76845.6\u500d\u3002\u7814\u7a76\u6210\u679c\u4ee5\u9898\u4e3a\u201cLight-Assisted CO2<\/sub> Hydrogenation over Pd3<\/sub>Cu@UiO-66 Promoted by Active Sites in Close Proximity\u201d<\/strong>\u53d1\u5e03\u5728\u56fd\u9645\u8457\u540d\u671f\u520aAngew. Chem. Int. Ed.<\/strong>\u4e0a\u3002 \u56fe\u4e00\u3001Pd3<\/sub>Cu@UiO-66\u548cPd3<\/sub>Cu\/UiO-66\u4e0a\u5149\u8f85\u52a9CO2<\/sub>\u52a0\u6c22\u6210CH3<\/sub>OH\u7684\u793a\u610f\u56fe<\/strong><\/p>\n \uff08c-f\uff09\u9ad8\u5206\u8fa8\u900f\u5c04\u7535\u955c\u56fe\u7247\u548c\u76f8\u5e94\u7684Zr\u3001Pd\u3001Cu\u5143\u7d20\u626b\u63cf\u56fe\u7247\u3002<\/p>\n \u56fe\u4e09\u3001Pd3<\/sub>Cu@UiO-66\u4e0a\u7684\u5149\u8f85\u52a9CO2<\/sub>\u5408\u6210\u7532\u9187<\/strong> \uff08b-c\uff09Pd3<\/sub>Cu@UiO-66\u7684\u963f\u4f26\u5c3c\u4e4c\u65af\u56fe\u548c\u52a8\u529b\u5b66\u66f2\u7ebf\uff1b<\/p>\n \uff08d\uff09Pd3<\/sub>Cu@UiO-66\u7684\u50ac\u5316\u5faa\u73af\u6d4b\u8bd5\u3002<\/p>\n \u56fe\u56db\u3001CO2<\/sub>-TPD\u548cH2<\/sub>-TPD\u6d4b\u8bd5<\/strong> \u56fe\u4e94\u3001Pd3<\/sub>Cu@UiO-66\u4e0aCO2<\/sub>\u52a0\u6c22\u5236\u7532\u9187\u7684\u6027\u80fd\u6d4b\u8bd5\u4e0e\u8868\u5f81<\/strong> \uff08b\uff09\u4e0d\u540c\u6ce2\u957f\u4e0b\u7684\u7684\u7532\u9187\u5408\u6210\u4ea7\u7387\uff1b<\/p>\n \uff08c\uff09UiO-66\u548cPd3<\/sub>Cu@UiO-66\u7684\u7d2b\u5916-\u53ef\u89c1\u5438\u6536\u5149\u8c31\uff1b<\/p>\n \uff08d\uff09Pd3<\/sub>Cu@UiO-66\u5728\u4e0d\u540c\u6761\u4ef6\u4e0b\u7684ESR\u8c31\u3002<\/p>\n \u56fe\u516d\u3001\u539f\u4f4dDRIFT\u5149\u8c31<\/strong> \uff08b\uff09\u5438\u9644\u5728\u5f00\u653eZr\u4f4d\u70b9\u4e0a\u7684\u53cc\u9f7f\u7532\u9178\u76d0\u7269\u79cd\u7684\u03bd(C-H)\u3002<\/p>\n \u56fe\u4e03\u3001DFT\u8ba1\u7b97<\/strong> \uff08b\uff09CO2<\/sub>\u6c22\u5316\u53cd\u5e94\u8def\u5f84\u7684\u81ea\u7531\u80fd\u53d8\u5316\u3002<\/p>\n \u3010\u5c0f\u7ed3\u3011<\/strong><\/p>\n \u7efc\u4e0a\u6240\u8ff0\uff0c\u4f5c\u8005\u901a\u8fc7\u5c06\u8d85\u5c0f\u7684Pd3<\/sub>Cu NPs\u5747\u5300\u5730\u5c01\u88c5\u5728UiO-66\u4e2d\u5f97\u5230\u4e86Pd3<\/sub>Cu@UiO-66\u590d\u5408\u6750\u6599\uff0c\u5728\u5149\u7167\u5c04\u4e0b\u5c06CO2<\/sub>\u52a0\u6c22\u8f6c\u53d8\u4e3a\u7532\u9187\u4e2d\u8868\u73b0\u51fa\u4f18\u5f02\u7684\u50ac\u5316\u6d3b\u6027\u3002\u5149\u7167\u4e0b\uff0cUiO-66\u7684\u914d\u4f53\u6355\u83b7\u5149\u5b50\u5e76\u4ea7\u751f\u5149\u751f\u7535\u5b50\uff0c\u5149\u751f\u7535\u5b50\u901a\u8fc7LCCT\uff08\u914d\u4f53\u5230\u7c07\u7684\u7535\u8377\u8f6c\u79fb\uff09\u8fc7\u7a0b\u5c06\u5149\u751f\u7535\u5b50\u6ce8\u5165\u5230\u5438\u9644\u5728Zr-oxo\u7c07\u4e0a\u7684CO2<\/sub>\u7684\u53cd\u952e\u8f68\u9053\uff0c\u52a0\u901f\u4e86\u4e2d\u95f4\u7269\u79cdHCOO*\u7684\u751f\u6210\uff0c\u4ece\u800c\u663e\u8457\u964d\u4f4e\u4e86\u6574\u4e2a\u53cd\u5e94\u7684\u8868\u89c2\u6d3b\u5316\u80fd\u3002\u6d4b\u8bd5\u7ed3\u679c\u8868\u660e\uff0c\u5f53\u53cd\u5e94\u6761\u4ef6\u4e3a200 \u2103\u30011.25 MPa\uff0c\u5149\u7167\u4e0b\u7532\u9187\u7684\u6700\u5927\u4ea7\u7387\u4e3a340 \u00b5mol g-1<\/sup> h-1<\/sup>\uff0c\u6bd4\u9ed1\u6697\u4e2d\u7684\u4ea7\u7387\u9ad8\u51fa5.6\u500d\u3002\u6b64\u5916\uff0cPd3<\/sub>Cu\u76f8\u5bf9\u4e8eUiO-66\u7684\u7a7a\u95f4\u4f4d\u7f6e\u5728\u50ac\u5316\u4e2d\u8d77\u7740\u5173\u952e\u4f5c\u7528\u3002\u4e0ePd3<\/sub>Cu\/UiO-66\uff08Pd3<\/sub>Cu NPs\u5206\u6563\u5728UiO-66\u5b54\u5916\uff09\u76f8\u6bd4\uff0cPd3<\/sub>Cu@UiO-66\uff08Pd3<\/sub>Cu NPs\u5206\u6563\u5728UiO-66\u5b54\u5185\uff09\u4e2d\u9ad8\u5ea6\u5206\u6563\u7684Pd3<\/sub>Cu NPs\u4f7f\u5f97Zr-oxo\u7c07\u548cPd3<\/sub>Cu NPs\u7684\u6d3b\u6027\u4f4d\u70b9\u5341\u5206\u63a5\u8fd1\uff0c\u4f7fPd3<\/sub>Cu\u5411\u5468\u56f4\u7684Zr-oxo\u7c07\u63d0\u4f9b\u8db3\u591f\u7684\u6ea2\u6d41\u6c22\uff0c\u964d\u4f4e\u53cd\u5e94\u7684\u8868\u89c2\u6d3b\u5316\u80fd\u3002\u8be5\u5de5\u4f5c\u4e0d\u4ec5\u4e3a\u5149\u70ed\u534f\u540c\u50ac\u5316\u63d0\u4f9b\u4e86\u6df1\u5165\u4e86\u89e3\uff0c\u800c\u4e14\u8bc1\u660e\u4e86CO2<\/sub>\u548cH2<\/sub>\u6d3b\u5316\u4f4d\u70b9\u4e4b\u95f4\u7684\u8fd1\u90bb\u4f5c\u7528\u5728CO2<\/sub>\u52a0\u6c22\u4e2d\u7684\u91cd\u8981\u4f5c\u7528\u3002<\/p>\n
\n
\u3010\u6210\u679c\u7b80\u4ecb\u3011<\/strong><\/p>\n
\n
\u3010\u56fe\u6587\u89e3\u8bfb\u3011<\/strong><\/p>\n
\n \u56fe\u4e8c\u3001Pd3<\/sub>Cu@UiO-66\u7684\u7ed3\u6784\u8868\u5f81<\/strong>
\n
\uff08a-b\uff09Pd3<\/sub>Cu@UiO-66 TEM\u56fe\u7247\uff1b<\/p>\n
\n
\uff08a\uff09\u4e0d\u540c\u53cd\u5e94\u6e29\u5ea6\u4e0bCH3<\/sub>OH\u7684\u751f\u4ea7\u901f\u7387\uff1b<\/p>\n
\n
\uff08a-b\uff09Pd3<\/sub>Cu@UiO-66\u548cUiO-66\u7684CO2<\/sub>-TPD\u548cH2<\/sub>-TPD\u66f2\u7ebf\u3002<\/p>\n
\n
\uff08a\uff09\u4e0d\u540c\u5149\u7167\u5f3a\u5ea6\u4e0b\u7684\u7532\u9187\u5408\u6210\u4ea7\u7387\uff1b<\/p>\n
\n
\uff08a\uff09Pd3<\/sub>Cu@UiO-66\u57283500-2700 cm-1<\/sup>\u8303\u56f4\u5185\u7684\u539f\u4f4dDRIFT\u5149\u8c31\uff1b<\/p>\n
\n
\uff08a\uff09\u5438\u9644\u5728\u4e0d\u9971\u548cZr-oxo\u7c07\u4e0a\u7684\u4ea7\u7269\u4e2d\u95f4\u4f53\u6a21\u578b\uff1b<\/p>\n