{"id":229371,"date":"2021-11-11T12:30:15","date_gmt":"2021-11-11T04:30:15","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=229371"},"modified":"2021-11-11T12:00:53","modified_gmt":"2021-11-11T04:00:53","slug":"%ef%bc%88%e5%b7%b2%e6%a0%a1%e7%a8%bf%e4%bb%b6%ef%bc%89%e5%8d%97%e4%ba%ac%e5%b8%88%e5%a4%a7%e5%85%b0%e4%ba%9a%e4%b9%be-nat-commun-%ef%bc%9acmof%e8%b4%9f%e8%bd%bd%e5%8d%95cu%e4%bd%8d%e7%82%b9%e5%8a%a9","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=229371","title":{"rendered":"\u5357\u4eac\u5e08\u5927\u5170\u4e9a\u4e7e Nat. Commun.\uff1acMOF\u8d1f\u8f7d\u5355Cu\u4f4d\u70b9\u52a9\u529bCO2\u8fd8\u539f\u4e3aCH4"},"content":{"rendered":"

\u3010\u80cc\u666f\u4ecb\u7ecd\u3011<\/strong><\/p>\n

\u901a\u8fc7\u7535\u50ac\u5316\u5c06\u4e3b\u8981\u6e29\u5ba4\u6c14\u4f53\u4e8c\u6c27\u5316\u78b3\uff08CO2<\/sub>\uff09\u6709\u6548\u8fd8\u539f\u4e3a\u5316\u5b66\u54c1\uff0c\u6709\u52a9\u4e8e\u51cf\u5c11\u6c14\u5019\u53d8\u5316\u7684\u5f71\u54cd\u4ee5\u53ca\u7f13\u89e3\u80fd\u6e90\u5371\u673a\u5177\u6709\u91cd\u5927\u610f\u4e49\u3002\u7535\u5316\u5b66CO2<\/sub>\u8fd8\u539f\uff08ECR\uff09\u4e3aC2<\/sub>H4<\/sub>\u3001CH4<\/sub>\u7b49\u78b3\u6c22\u5316\u5408\u7269\u5177\u6709\u5e7f\u9614\u7684\u524d\u666f\uff0c\u4f46ECR\u5b58\u5728\u52a8\u529b\u5b66\u7f13\u6162\u548c\u526f\u53cd\u5e94\u5bfc\u81f4\u4f4e\u9009\u62e9\u6027\u3001\u65e0\u6d3b\u6027\u548c\u8010\u4e45\u6027\u6709\u9650\u7684\u95ee\u9898\u3002\u6b64\u5916\uff0c\u7531\u4e8e\u6790\u6c22\u53cd\u5e94\uff08HER\uff09\u7684\u5e72\u6270\u548c\u53cd\u5e94\u8fc7\u7a0b\u4e2d\u6d89\u53ca\u7684\u591a\u4e2a\u7535\u5b50\u8f6c\u79fb\u8fc7\u7a0b\uff0cECR\u5bf9\u78b3\u6c22\u5316\u5408\u7269\u7684\u9009\u62e9\u6027\u8f83\u4f4e\u3002\u76ee\u524d\uff0c\u94dc\uff08Cu\uff09\u57fa\u7535\u50ac\u5316\u5242\u80fd\u6709\u6548\u4fc3\u8fdbECR\u8f6c\u5316\u4e3a\u78b3\u6c22\u5316\u5408\u7269\uff0c\u4f46\u4ecd\u5b58\u5728\u9009\u62e9\u6027\u8f83\u4f4e\u95ee\u9898\u3002\u5355\u4f4d\u70b9\u50ac\u5316\u5242\uff08SSCs\uff09\u53ef\u4ee5\u5b9e\u73b0\u9ad8\u9009\u62e9\u6027\u7cbe\u786e\u50ac\u5316\uff0c\u4f46\u662f\u5927\u591a\u6570\u5df2\u62a5\u9053\u7684\u5355\u539f\u5b50\u50ac\u5316\u5242\u66f4\u6709\u5229\u4e8e\u5f62\u6210\u53cc\u7535\u5b50\u4ea7\u7269\uff08CO\uff09\u3002\u540c\u65f6\uff0c\u9664\u6c2e\u914d\u4f4d\u7684\u5355\u539f\u5b50\u4f4d\u70b9\u5916\uff0c\u5f88\u5c11\u7814\u7a76\u62a5\u9053\u5176\u5b83\u6742\u539f\u5b50\u914d\u4f4d\u7684\u5355\u91d1\u5c5e\u4f4d\u70b9\u3002\u5bfc\u7535\u91d1\u5c5e\u6709\u673a\u9aa8\u67b6\uff08cMOF\uff09\u6750\u6599\u662f\u7531\u5177\u6709\u5171\u8f6d\u6709\u673a\u914d\u4f53\u7684\u8fc7\u6e21\u91d1\u5c5e\u79bb\u5b50\u81ea\u7ec4\u88c5\u800c\u6210\uff0c\u6709\u72ec\u7279\u7684\u6c27\u5316\u8fd8\u539f\u548c\u5bfc\u7535\u6027\u4ee5\u53caMOF\u57fa\u7684\u6027\u8d28\u3002\u7136\u800c\uff0c\u5bf9\u4e8ecMOF\u7535\u50ac\u5316\u5242\u7684\u7814\u7a76\u4ecd\u7136\u5f88\u5c11\u3002
\n \"\"\u3010\u6210\u679c\u7b80\u4ecb\u3011<\/strong><\/p>\n

\u8fd1\u65e5\uff0c\u5357\u4eac\u5e08\u8303\u5927\u5b66\u5170\u4e9a\u4e7e\u6559\u6388\uff08\u901a\u8baf\u4f5c\u8005\uff09\u7b49\u4eba<\/strong>\u62a5\u9053\u4e86\u4e00\u79cd\u7531\u9ad8\u5ea6\u5171\u8f6d\u7684\u7c7b\u77f3\u58a8\u70ef\u914d\u4f53\uff08\u4e8c\u82ef\u5e76[g, p]chrysene-2, 3, 6, 7, 10, 11, 14, 15-\u8f9b\u9187\uff0c8OH-DBC\uff09\u548cCu\u4f4d\u70b9\u7ec4\u6210\u7684Cu-\u57fa\u5bfc\u7535\u91d1\u5c5e\u6709\u673a\u9aa8\u67b6\uff08cMOF\uff09\uff08\u7b80\u5199\u4e3aCu-DBC\uff09\uff0c\u5e76\u5c06\u5176\u4f5c\u4e3aCO2<\/sub>\u8fd8\u539f\u4e3a\u7532\u70f7\uff08CH4<\/sub>\uff09\u7684\u9ad8\u6548\u7535\u50ac\u5316\u5242\u3002\u901a\u8fc7\u673a\u7406\u7814\u7a76\u53d1\u73b0\uff0c\u9ad8\u5ea6\u5171\u8f6d\u7684\u6709\u673a\u914d\u4f53\u4f7f\u5f97Cu-DBC\u5177\u6709\u72ec\u7279\u7684\u6c27\u5316\u8fd8\u539f\u6027\u80fd\u548c\u5bfc\u7535\u6027\uff0c\u800c\u4e30\u5bcc\u4e14\u5747\u5300\u5206\u5e03\u7684Cu-O4<\/sub>\u4f4d\u70b9\u4f7f\u5176\u53ef\u4ee5\u9ad8\u9009\u62e9\u6027\u7684\u8fdb\u884c\u9ad8\u6548ECR\u8f6c\u5316\u4e3aCH4<\/sub>\u8fc7\u7a0b\u3002\u5b9e\u9a8c\u6d4b\u8bd5\u53d1\u73b0\uff0c\u5728-0.9 V vs RHE\u7684\u4f4e\u8fd8\u539f\u7535\u4f4d\u4e0b\uff0cCu-DBC\u8868\u73b0\u51fa\u7ea680%\u7684\u9ad8CH4<\/sub> FE\u3001\u5c40\u90e8\u7535\u6d41\u5bc6\u5ea6\u4e3a-162.4 mA cm-2<\/sup>\uff0c\u8fd9\u662f\u5c06CO2<\/sub>\u8fd8\u539f\u4e3aCH4<\/sub>\u7684\u6700\u4f73Cu\u57fa\u7535\u50ac\u5316\u5242\u4e4b\u4e00\u3002\u6b64\u5916\uff0c\u57fa\u4e8e\u7ed3\u6676\u591a\u5b54\u50ac\u5316\u5242\u5177\u6709\u660e\u786e\u7684\u7ed3\u6784\uff0c\u4f5c\u8005\u8fd8\u7814\u7a76\u4e86\u5355\u4e2aCu\u4f4d\u70b9\u7684\u914d\u4f4d\u73af\u5883\u4e0e\u7535\u5316\u5b66\u8fd8\u539f\u50ac\u5316\u9009\u62e9\u6027\u4e4b\u95f4\u7684\u5173\u7cfb\u3002\u901a\u8fc7\u7535\u50ac\u5316\u6d4b\u91cf\u548c\u8ba1\u7b97\u7814\u7a76\uff0c\u4f5c\u8005\u8fdb\u4e00\u6b65\u7cfb\u7edf\u5730\u7814\u7a76\u4e86Cu-DBC\u50ac\u5316\u5242\u5bf9ECR\u8f6c\u5316\u4e3aCH4<\/sub>\u53cd\u5e94\u7684\u7279\u6b8a\u6027\u548c\u8be6\u7ec6\u7684\u50ac\u5316\u673a\u7406\u3002\u8be5\u7814\u7a76\u4e3a\u8bbe\u8ba1\u5177\u6709\u660e\u786e\u7ed3\u6784\u7684ECR\u50ac\u5316\u5242\u63d0\u4f9b\u4e86\u4e00\u79cd\u7b56\u7565\uff0c\u5e76\u4e3a\u6784\u5efa\u9ad8\u6548ECR\u50ac\u5316\u5242\u7684\u7cbe\u786e\u7ed3\u6784-\u53cd\u5e94\u76f8\u5173\u6027\u5960\u5b9a\u4e86\u57fa\u7840\u3002\u7814\u7a76\u6210\u679c\u4ee5\u9898\u4e3a\u201cCoordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2<\/sub> reduction to CH4<\/sub>\u201d<\/strong>\u53d1\u5e03\u5728\u56fd\u9645\u8457\u540d\u671f\u520aNature Communications<\/strong>\u4e0a\u3002<\/p>\n

\u3010\u56fe\u6587\u89e3\u8bfb\u3011<\/strong><\/p>\n

\u56fe\u4e00\u3001Cu-DBC\u7535\u50ac\u5316\u5242\u7684\u8868\u5f81<\/strong>
\n \"\"\uff08a\uff09\u7531\u94dc\u79bb\u5b50\u548c8OH-DBC\u5408\u6210\u5f97\u5230\u7684\u7ed3\u6784\u793a\u610f\u56fe\uff1b<\/p>\n

\uff08b\uff09\u6a21\u62df\u548c\u5b9e\u9a8c\u5f97\u5230PXRD\u56fe\u6848\uff1b<\/p>\n

\uff08c\uff09\u5229\u7528\u56db-\u63a5\u89e6\u63a2\u9488\u65b9\u6cd5\u7684\u7535\u6d41-\u7535\u538b\u66f2\u7ebf\u56fe\uff1b<\/p>\n

\uff08d\uff09TEM\u56fe\u50cf\uff1b<\/p>\n

\uff08e\uff09STEM\u56fe\u50cf\u548c\u76f8\u5e94\u7684Cu\u3001C\u548cO\u5143\u7d20\u6620\u5c04\u56fe\u50cf\u3002<\/p>\n

\u56fe\u4e8c\u3001Cu-DBC\u7535\u50ac\u5316\u5242\u7684ECR\u8f6c\u5316\u4e3aCH4<\/sub>\u6027\u80fd<\/strong>
\n \"\"\uff08a\uff09\u5728CO2<\/sub>\u548cAr\u4e0b\u8bb0\u5f55\u7684\u6781\u5316\u66f2\u7ebf\uff1b<\/p>\n

\uff08b\uff09ECR\u4ea7\u7269\u5728\u4e0d\u540c\u5e94\u7528\u7535\u4f4d\u4e0b\u7684\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FE\uff09\uff1b<\/p>\n

\uff08c\uff09\u5728\u4e0d\u540c\u65bd\u52a0\u7535\u4f4d\u4e0b\uff0c\u8bb0\u5f55\u7684HER\u3001ECR\u548cCH4<\/sub>\u7684FE\uff1b<\/p>\n

\uff08d\uff09\u5728-0.9 V vs RHE\u7684\u6052\u5b9a\u7535\u538b\u4e0b\uff0cCH4<\/sub>\u7684\u7535\u6d41\u5206\u5e03\u548cFE\uff1b<\/p>\n

\uff08e\uff09\u572813<\/sup>CO2<\/sub>\u6c14\u6c1b\u4e0b\u8bb0\u5f55\u768413<\/sup>CH4<\/sub>\u7684\u8d28\u8c31\u56fe\uff1b<\/p>\n

\uff08f\uff09\u65b0\u5236\u548c\u6d4b\u8bd5\u8fc7\u7684Cu-DBC\u6539\u6027GDL-\u78b3\u7eb8\u7535\u6781\u7684XRD\u56fe\u6848\u3002<\/p>\n

\u56fe\u4e09\u3001\u6676\u4f53\u5355\u4f4d\u70b9Cu\u7535\u50ac\u5316\u5242\u7684ECR\u6027\u80fd<\/strong>
\n \"\"\uff08a\uff09\u4e0d\u540cCu\u57fa\u50ac\u5316\u5242\u7ed3\u6784\u793a\u610f\u56fe\uff1b<\/p>\n

\uff08b\uff09\u4e0d\u540cCu\u57fa\u50ac\u5316\u5242\u7684LSV\u6781\u5316\u66f2\u7ebf\uff1b<\/p>\n

\uff08c\uff09\u5728\u4e0d\u540c\u65bd\u52a0\u7535\u4f4d\u4e0b\uff0c\u4e0d\u540cCu\u57fa\u50ac\u5316\u5242\u7684CH4<\/sub>\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FE\uff09\uff1b<\/p>\n

\uff08d\uff09\u4e0d\u540cCu\u57fa\u50ac\u5316\u5242\u7684\u5c40\u90e8CH4<\/sub>\u7535\u6d41\u5bc6\u5ea6\uff1b<\/p>\n

\uff08e\uff09\u5728-0.9 V vs RHE\u4e0b\uff0c\u4e0d\u540cCu\u57fa\u50ac\u5316\u5242\u7684\u6574\u4f53ECR\u6027\u80fd\u8bc4\u4f30\u3002<\/p>\n

\u56fe\u56db\u3001ECR\u9009\u62e9\u6027\u5bf9Cu\u4f4d\u914d\u4f4d\u73af\u5883\u7684\u4f9d\u8d56\u6027<\/strong>
\n \"\"\uff08a\uff09Cu-DBC\u3001Cu-TTCOF\u548cCu-PPCOF\u50ac\u5316\u5242\u4e2dCu-O4<\/sub>\u3001\u535f\u5549Cu-N4<\/sub>\u548c\u915e\u83c1Cu-N4<\/sub>\u4f4d\u70b9\u7684DFT\u8ba1\u7b97\u6a21\u578b\u793a\u610f\u56fe\uff1b<\/p>\n

\uff08b\uff09\u5728-0.9 V vs. RHE\u4e0b\uff0c\u4e0d\u540c\u7684\u5355Cu\u4f4d\u70b9\u7535\u50ac\u5316\u5242\u4e0a\u7684ECR\u548cHER\u7684FE\u8bb0\u5f55\u503c\uff1b<\/p>\n

\uff08c\uff09\u901a\u8fc7DFT\u8ba1\u7b97\uff0c*H\u5438\u9644\u5728\u4e0d\u540c\u50ac\u5316\u4f4d\u70b9\u4e0a\u7684\u80fd\u91cf\u5206\u5e03\uff1b<\/p>\n

\uff08d\uff09\u4eceECR\u5230CH4<\/sub>\u53cd\u5e94\u9014\u5f84\u7684\u81ea\u7531\u80fd\u5206\u5e03\u3002<\/p>\n

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

\u7efc\u4e0a\u6240\u8ff0\uff0c\u672c\u6587\u4e3aCu\u57facMOF\u7684CO2<\/sub>\u8fd8\u539f\u63d0\u4f9b\u4e86\u4e00\u79cd\u7535\u50ac\u5316\u5242\u3002\u5236\u5907\u7684Cu-DBC\u5177\u6709\u5206\u6563\u7684\u5355Cu\u4f4d\u70b9\u548c\u5747\u5300\u7684\u5fae\u5b54\uff0c\u5177\u6709\u826f\u597d\u7684\u6c27\u5316\u8fd8\u539f\u6027\u80fd\u548cCO2<\/sub>\u5438\u9644\u80fd\u529b\u3002\u5728\u4e0eGDL\u7ed3\u5408\u540e\uff0cCu-DBC\u50ac\u5316\u5242\u5728-0.9 V vs RHE\u4e0b\u5bf9CH4\u5177\u6709\u7ea680%\u7684\u9ad8\u9009\u62e9\u6027\uff0c\u5e76\u4e14\u5728\u6d41\u52a8\u6c60\u4e2d\u6d4b\u8bd5\u65f6\u5177\u6709\u7ea6-203 mA cm-2<\/sup>\u7684\u9ad8\u50ac\u5316\u7535\u6d41\u5bc6\u5ea6\uff0c\u8fd9\u662f\u76ee\u524d\u6700\u5148\u8fdb\u7684ECR\u8f6c\u5316\u4e3aCH4<\/sub>\u50ac\u5316\u5242\u4e4b\u4e00\u3002\u901a\u8fc7DFT\u8ba1\u7b97\u548c\u7535\u50ac\u5316\u6d4b\u91cf\uff0c\u4f5c\u8005\u7814\u7a76\u4e86ECR\u9009\u62e9\u6027\u4e0e\u5355Cu\u4f4d\u70b9\u914d\u4f4d\u73af\u5883\u4e4b\u95f4\u7684\u76f8\u5173\u6027\u3002\u5bf9\u6bd4\u6c2e\u914d\u4f4dCu\u4f4d\u70b9\uff0c\u4f4e\u53cd\u5e94\u80fd\u5792Cu-DBC\u4e2d\u7684Cu-O4<\/sub>\u4f4d\u70b9\u5177\u6709\u66f4\u597d\u7684ECR\u6027\u80fd\u3002\u672c\u6587\u6240\u63d0\u51fa\u7684\u5bfc\u7535MOF\u7684\u8bbe\u8ba1\u53ef\u4e3a\u66f4\u597d\u5730\u7406\u89e3ECR\u7684\u50ac\u5316\u5242\u7ed3\u6784\u548c\u7535\u5316\u5b66\u6027\u80fd\u4e4b\u95f4\u7684\u76f8\u5173\u6027\u5960\u5b9a\u7406\u8bba\u548c\u5b9e\u9a8c\u57fa\u7840\uff0c\u4ee5\u4fbf\u8fdb\u4e00\u6b65\u7814\u7a76\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1aCoordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2<\/sub> reduction to CH4<\/sub><\/a><\/strong>. Nat. Commun.<\/em>, 2021<\/strong>, DOI: 10.1038\/s41467-021-26724-8.<\/p>\n

\u672c\u6587\u7531CQR\u7f16\u8bd1\u3002<\/p>\n

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