{"id":132036,"date":"2018-04-01T06:30:21","date_gmt":"2018-03-31T22:30:21","guid":{"rendered":"\/\/m.iemloyee.com\/?p=132036"},"modified":"2018-04-01T11:13:42","modified_gmt":"2018-04-01T03:13:42","slug":"j-am-chem-soc-%ef%bc%9aco-n5-%e5%8d%95%e5%8e%9f%e5%ad%90%e5%82%ac%e5%8c%96%e4%bd%8d%e7%82%b9%e7%9a%84%e8%ae%be%e8%ae%a1-%e6%8e%a5%e8%bf%91100co%e9%80%89%e6%8b%a9%e6%80%a7%e4%bb%a5","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=132036","title":{"rendered":"J. Am. Chem. Soc.\uff1aCo-N5 \u5355\u539f\u5b50\u50ac\u5316\u4f4d\u70b9\u7684\u8bbe\u8ba1\u2014\u2014\u63a5\u8fd1100%CO\u9009\u62e9\u6027\u4ee5\u53ca\u51fa\u8272\u7684\u7a33\u5b9a\u6027\u7684\u7535\u50ac\u5316\u8fd8\u539fCO2\u50ac\u5316\u5242"},"content":{"rendered":"

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

\u7535\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u662fCO2<\/sub>\u8f6c\u6362\u662f\u4e00\u4e2a\u91cd\u8981\u7684\u8fc7\u7a0b\uff0c\u80fd\u591f\u5728\u6e29\u548c\u7684\u53cd\u5e94\u6761\u4ef6\u4e0b\u5c06CO2<\/sub>\u4e00\u6b65\u8f6c\u5316\u4e3aCO\u3001HCOOH\u3001\u78b3\u6c22\u5316\u5408\u7269\u548c\u9187\u7c7b\u7b49\u9ad8\u9644\u52a0\u503c\u71c3\u6599\u53ca\u5316\u5b66\u54c1\uff0c\u540c\u65f6\u5b9e\u73b0\u4e8c\u6c27\u5316\u78b3\u7684\u9ad8\u6548\u8f6c\u5316\u3002\u4f46\u662f\uff0c\u8be5\u8fc7\u7a0b\u5b58\u5728\u7ade\u4e89\u7684\u6790\u6c22\u53cd\u5e94\uff0c\u540c\u65f6\u9ad8\u7684\u8fc7\u7535\u4f4d\u964d\u4f4e\u4e86\u4ea7\u7269\u7684\u9009\u62e9\u6027\u4ee5\u53ca\u8f6c\u6362\u6548\u7387\u3002\u7814\u7a76\u8868\u660e\u4e00\u7cfb\u5217\u7684\u7535\u50ac\u5316\u5242\u5305\u62ec\u91d1\u5c5e\u3001\u5408\u91d1\u4ee5\u53ca\u5206\u5b50\u5316\u5408\u7269\u7b49\u88ab\u7528\u6765\u63d0\u9ad8\u7535\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u6d3b\u6027\u3002\u5728\u8fd9\u4e9b\u6750\u6599\u4e2d\uff0c\u7531\u4e8e\u91d1\u5c5e\u535f\u5549\u548c\u915e\u83c1\u7c7b\u5177\u6709\u6e05\u6670\u7684\u5206\u5b50\u7ed3\u6784\u4ee5\u53ca\u539f\u5b50\u7ed3\u6784\u7684\u53ef\u8c03\u8282\u6027\uff0c\u88ab\u8ba4\u4e3a\u662f\u63a2\u7d22\u50ac\u5316\u673a\u5236\u4ee5\u53ca\u4f18\u5316\u50ac\u5316\u6d3b\u6027\u7684\u7406\u60f3\u6a21\u578b\u3002\u8fd1\u5e74\u6765\uff0c\u6c2e\u63ba\u6742\u78b3\u6750\u6599\u951a\u5b9a\u91d1\u5c5e\u5355\u539f\u5b50\u50ac\u5316\u5242\u53d7\u5230\u4e86\u5e7f\u5927\u79d1\u7814\u4eba\u5458\u7684\u5173\u6ce8\u4e0e\u7814\u7a76\uff0c\u5e76\u4e14\u5176\u7279\u6b8a\u7684\u7535\u5b50\u7ed3\u6784\u548c\u6700\u5927\u7684\u539f\u5b50\u5316\u5229\u7528\u4f7f\u5b83\u4eec\u80fd\u591f\u4f5c\u4e3a\u9ad8\u6548\u7684CO2<\/sub>\u8fd8\u539f\u50ac\u5316\u5242\u3002\u5c3d\u7ba1\u7814\u7a76\u4eba\u5458\u8fdb\u884c\u4e86\u5e7f\u6cdb\u7684\u7814\u7a76\uff0c\u8bbe\u8ba1\u9ad8\u6548\u50ac\u5316\u5242\u6765\u964d\u4f4e\u8fc7\u7535\u52bf\u548c\u63d0\u9ad8\u53cd\u5e94\u9009\u62e9\u6027\u4ee5\u53ca\u63a2\u7d22\u50ac\u5316\u6d3b\u6027\u4e2d\u5fc3\u4ecd\u7136\u662f\u7535\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u7814\u7a76\u4e2d\u6781\u5177\u6311\u6218\u6027\u7684\u70ed\u70b9\u8bfe\u9898\u3002<\/p>\n

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

\u8fd1\u65e5\uff0c\u6765\u81ea\u6e05\u534e\u5927\u5b66\u7684\u9648\u6668\u6559\u6388\uff08\u901a\u8baf\u4f5c\u8005\uff09<\/strong>\u56e2\u961f\u5728J. Am. Chem. Soc.<\/strong>\u53d1\u6587\uff0c\u9898\u4e3a\uff1a\u201cDesign of Single-Atom Co-N5 <\/sub>Catalytic Site: A Robust Electrocatalyst for CO2<\/sub> Reduction with Nearly 100% CO Selectivity and Remarkable Stability<\/strong>\u201d\u3002\u7814\u7a76\u4eba\u5458\u91c7\u7528\u4e86\u4e00\u79cd\u6c2e\u914d\u4f4d\u7b56\u7565\u6765\u8bbe\u8ba1\u5728\u805a\u5408\u7269\u884d\u751f\u7684\u7a7a\u5fc3\u6c2e\u63ba\u6742\u591a\u5b54\u78b3\u7403\u4e0a\u5177\u6709\u539f\u5b50\u7ea7\u5206\u6563\u7684Co-N5<\/sub>\u4f4d\u70b9\u7684\u9ad8\u6548\u7684CO2<\/sub>\u8fd8\u539f\u7535\u50ac\u5316\u5242\u3002\u8be5\u50ac\u5316\u5242\u5728\u7535\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u53cd\u5e94\u4e2d\u8868\u73b0\u51fa\u9ad8\u7684\u6d3b\u6027\u548c\u9009\u62e9\u6027\uff0c\u5176CO\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FECO<\/sub>\uff09\u5728-0.57V\u5230-0.88V\u8fd9\u4e2a\u5bbd\u7535\u4f4d\u8303\u56f4\u5185\u5747\u5927\u4e8e90%\uff0c\u5e76\u4e14\u5728-0.73V\u548c-0.79V\u4e0bFECO<\/sub>\u5927\u4e8e99%\u3002\u7a33\u5b9a\u6027\u6d4b\u8bd5\u7ed3\u679c\u8868\u660e\uff0c\u7ecf\u8fc710\u5c0f\u65f6\uff0cCO\u7684\u7535\u6d41\u5bc6\u5ea6\u4ee5\u53caFECO<\/sub>\u51e0\u4e4e\u6ca1\u6709\u8870\u51cf\uff0c\u8bc1\u660e\u8be5\u50ac\u5316\u5242\u975e\u5e38\u7a33\u5b9a\u3002\u5b9e\u9a8c\u548cDFT\u8ba1\u7b97\u8bc1\u660e\u5355\u539f\u5b50Co-N5<\/sub>\u4f4d\u70b9\u662f\u50ac\u5316\u6d3b\u6027\u4e2d\u5fc3\uff0c\u540c\u65f6\u4e5f\u662f\u4e2d\u95f4\u4ea7\u7269COOH*\u5feb\u901f\u751f\u6210\u4ee5\u53caCO\u8131\u9644\u7684\u5173\u952e\u3002<\/p>\n

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

\u56fe1. \u7ed3\u6784\u8868\u5f81<\/strong><\/p>\n

\"\"<\/p>\n

(a) \u5408\u6210\u793a\u610f\u56fe\uff1b<\/p>\n

(b) SEM\uff1b<\/p>\n

(c) TEM\uff1b<\/p>\n

(d) HAADF STEM\u548cEDS\u56fe, C (\u84dd), N (\u7eff)\uff0cCo (\u7ea2)\uff1b<\/p>\n

(e, f) AC HAADF-STEM\u548c\u653e\u5927\u56fe\u50cf\uff1b.<\/p>\n

\u56fe2. XANES\u56fe<\/strong><\/p>\n

\"\"<\/p>\n

(a) Co K-\u8fb9: Co\u7b94, CoO, Co3<\/sub>O4<\/sub>, CoPc, Co-N5<\/sub>\/HNPCSs\uff1b<\/p>\n

(b) Co-N5<\/sub>\/HNPCSs\u50ac\u5316\u5242\u5728\u4e0d\u540c\u70ed\u89e3\u6e29\u5ea6\u4e0b\u7684Co K-\u8fb9(\u63d2\u56fe\u4e3a\u653e\u5927\u56fe)\uff1b<\/p>\n

(c) WT\uff1b<\/p>\n

(d)\u5728R\u7a7a\u95f4\u7684FT\uff1b<\/p>\n

(e) \u7b80\u5355\u7684\u7ed3\u6784\u6a21\u578b, Co (\u6d45\u84dd), N (\u84dd), C (\u7070) H (\u767d)\uff1b<\/p>\n

\u56fe3. \u7535\u50ac\u5316CO2<\/sub>\u8fd8\u539f\u6027\u80fd<\/strong><\/p>\n

\"\"<\/p>\n

(a) LSV\u66f2\u7ebf\uff1b<\/p>\n

(b) Co-5<\/sub>\/HNPCSs\u548cCoPc\u7684FECO<\/sub>\u548cFEH2<\/sub>\u5bf9\u6bd4\uff1b<\/p>\n

(c) M-N5<\/sub>\/HNPCSs (M = Co, Fe, Ni, Cu)\u7684FECO<\/sub>\u548cFEH2<\/sub>\uff1b<\/p>\n

(d) Co-N5<\/sub>\/HNPCSs-T\u7684FECO<\/sub>\u548cFEH2<\/sub>\uff1b<\/p>\n

(e) \u5728-0.73 V\u7684\u8ba1\u65f6\u7535\u6d41(\u63d2\u56fe\u662f\u5728\u4e0d\u540c\u65f6\u95f4\u7684FECO<\/sub>\u548cFEH2<\/sub>)\uff1b<\/p>\n

(f) Co-N5<\/sub>\/HNPCSs\u50ac\u5316\u5242\u5728\u975e\u539f\u4f4d\u548c\u539f\u4f4d\u4e0b\u7684XANES\u56fe(\u63d2\u56fe\u4e3a\u653e\u5927\u56fe)\uff1b<\/p>\n

\u56fe4. DFT\u8ba1\u7b97<\/strong><\/p>\n

\"\"<\/p>\n

(a) \u4e2d\u95f4\u4ea7\u7269\u7684\u4f18\u5316\u7ed3\u6784\uff1b<\/p>\n

(b) CO2<\/sub>\u8fd8\u539f\u81ea\u7531\u80fd\u8ba1\u7b97\uff1b<\/p>\n

\u3010\u603b\u7ed3\u3011<\/strong><\/p>\n

\u7814\u7a76\u4eba\u5458\u91c7\u7528\u4e86\u4e00\u79cd\u6c2e\u914d\u4f4d\u7b56\u7565\u8bbe\u8ba1\u4e86\u5728\u805a\u5408\u7269\u884d\u751f\u7684\u7a7a\u5fc3\u6c2e\u63ba\u6742\u591a\u5b54\u78b3\u7403\u4e0a\u5177\u6709\u539f\u5b50\u7ea7\u5206\u6563\u7684Co-N5<\/sub>\u4f4d\u70b9\u7684\u9ad8\u6548\u7684CO2<\/sub>\u8fd8\u539f\u7535\u50ac\u5316\u5242\u3002\u7814\u7a76\u53d1\u73b0\u5f62\u6210\u7684Co-N5<\/sub>\u4f4d\u70b9\u662f\u4e3b\u8981\u7684\u50ac\u5316\u6d3b\u6027\u4e2d\u5fc3\uff0c\u540c\u65f6\u4e5f\u662f\u4e2d\u95f4\u4ea7\u7269COOH*\u5feb\u901f\u751f\u6210\u4ee5\u53caCO\u8131\u9644\u7684\u5173\u952e\u3002\u8fd9\u9879\u5de5\u4f5c\u4e0d\u4ec5\u8bbe\u8ba1\u4e86\u4e00\u79cd\u9ad8\u6548\u7684\u4e8c\u6c27\u5316\u78b3\u8fd8\u539f\u7684\u7535\u50ac\u5316\u5242\u800c\u4e14\u4e5f\u5bf9\u50ac\u5316\u6d3b\u6027\u4e2d\u5fc3\u7684\u6df1\u5ea6\u7406\u89e3\u63d0\u4f9b\u4e86\u4e00\u4e2a\u65b0\u7684\u601d\u8def\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1a<\/strong>Design of Single-Atom Co\u2013N5<\/sub>\u00a0Catalytic Site: A Robust Electrocatalyst for CO2<\/sub> Reduction with Nearly 100% CO Selectivity and Remarkable Stability<\/a>, (J. Am. Chem. Soc., 2018, DOI:<\/strong>\u00a010.1021\/jacs.8b00814)<\/p>\n

\u672c\u6587\u7531\u6750\u6599\u4eba\u65b0\u80fd\u6e90\u5b66\u672f\u7ec4Z. Chen\u4f9b\u7a3f\uff0c\u6750\u6599\u725b\u6574\u7406\u7f16\u8f91\u3002<\/p>\n

\u6750\u6599\u725b\u7f51\u4e13\u6ce8\u4e8e\u8ddf\u8e2a\u6750\u6599\u9886\u57df\u79d1\u6280\u53ca\u884c\u4e1a\u8fdb\u5c55\uff0c\u8fd9\u91cc\u6c47\u96c6\u4e86\u5404\u5927\u9ad8\u6821\u7855\u535a\u751f\u3001\u4e00\u7ebf\u79d1\u7814\u4eba\u5458\u4ee5\u53ca\u884c\u4e1a\u4ece\u4e1a\u8005\uff0c\u5982\u679c\u60a8\u5bf9\u4e8e\u8ddf\u8e2a\u6750\u6599\u9886\u57df\u79d1\u6280\u8fdb\u5c55\uff0c\u89e3\u8bfb\u9ad8\u6c34\u5e73\u6587\u7ae0\u6216\u662f\u8bc4\u8ff0\u884c\u4e1a\u6709\u5174\u8da3\uff0c\u70b9\u6211\u52a0\u5165\u6750\u6599\u4eba\u7f16\u8f91\u90e8<\/a>\u3002<\/p>\n

\u6b22\u8fce\u5927\u5bb6\u5230\u6750\u6599\u4eba\u5ba3\u4f20\u79d1\u6280\u6210\u679c\u5e76\u5bf9\u6587\u732e\u8fdb\u884c\u6df1\u5165\u89e3\u8bfb\uff0c\u6295\u7a3f\u90ae\u7bb1\uff1atougao@cailiaoren.com\u3002<\/p>\n

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