{"id":228498,"date":"2021-10-16T06:30:34","date_gmt":"2021-10-15T22:30:34","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=228498"},"modified":"2021-10-15T15:29:59","modified_gmt":"2021-10-15T07:29:59","slug":"%e8%b4%b9%e6%85%a7%e9%be%99%e5%9b%a2%e9%98%9fchem-catalysis%ef%bc%9a%e5%af%8c%e8%be%b9%e7%bc%98%e7%bc%ba%e9%99%b7fen3%e4%bd%8d%e7%82%b9%e7%9a%84%e5%a4%9a%e5%ad%94fe-n-c%ef%bc%9a%e4%b8%80%e7%a7%8d","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=228498","title":{"rendered":"\u8d39\u6167\u9f99\u56e2\u961fChem\u00a0Catalysis\uff1a\u5bcc\u8fb9\u7f18\u7f3a\u9677FeN3\u4f4d\u70b9\u7684\u591a\u5b54Fe-N\/C\uff1a\u4e00\u79cd\u540c\u65f6\u5177\u5907\u9ad8\u672c\u5f81\u6d3b\u6027\u548c\u4f18\u5f02\u4f20\u8d28\u80fd\u529b\u7684\u9ad8\u6548ORR\u50ac\u5316\u5242\u00a0"},"content":{"rendered":"

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

\u5728\u71c3\u6599\u7535\u6c60\u548c\u91d1\u5c5e-\u7a7a\u6c14\u7535\u6c60\u7684\u53d1\u5c55\u4e2d\uff0c\u5927\u91cf\u7814\u7a76\u81f4\u529b\u4e8e\u5f00\u53d1\u975e\u8d35\u91d1\u5c5e-\u6c2e\/\u78b3\uff08M-N\/C\uff09\u50ac\u5316\u5242\u6765\u53d6\u4ee3\u6602\u8d35\u7684\u5546\u4e1a\u5316\u94c2\u78b3 (Pt\/C) \u7528\u4e8e\u9634\u6781\u6c27\u8fd8\u539f(ORR)\u53cd\u5e94\u3002\u5176\u4e2d\uff0c\u5355\u539f\u5b50\u50ac\u5316\u5242 (SACs) \u5177\u6709\u7406\u8bba\u4e0a\u539f\u5b50\u5229\u7528\u7387100%\u53ca\u53ef\u8c03\u7535\u5b50\u7ed3\u6784\u7b49\u4f18\u52bf\u800c\u5f15\u8d77\u5927\u91cf\u5173\u6ce8\u3002\u4f8b\u5982\uff0c\u5177\u6709\u5355\u5206\u6563Fe-N4<\/sub>\u4f4d\u70b9\u7684Fe-N\/C\u6750\u6599\u5df2\u88ab\u8bc1\u5b9e\u662f\u4e00\u79cd\u6bd4\u8f83\u6709\u6f5c\u529b\u7684ORR\u50ac\u5316\u5242\uff0c\u4f46\u7814\u7a76\u4e2d\u53d1\u73b0\u7531\u4e8e\u5927\u91cf\u5355\u539f\u5b50\u4f4d\u70b9\u88ab\u5305\u88f9\u5728\u50ac\u5316\u5242\u7684\u5fae\u5b54\u5185\u90e8\u800c\u672a\u53c2\u4e0e\u5230\u4e09\u76f8\u754c\u9762\u70b9\u4e0a\u5bfc\u81f4\u5b9e\u9645\u539f\u5b50\u5229\u7528\u7387\u4e00\u822c <5%\uff0c\u4ece\u800c\u4f7f\u5f97\u50ac\u5316\u6d3b\u6027\u8f83\u4f4e; \u800c\u4e14\uff0c\u90e8\u5206\u7814\u7a76\u62a5\u9053\u4f20\u7edf\u7684\u9762\u5185FeN4<\/sub>\u4f4d\u70b9\u7684Fe-N\/C\u50ac\u5316\u5242\u7684ORR\u6d3b\u6027\u53ef\u4ee5\u901a\u8fc7\u4f18\u5316\u5176\u7535\u5b50\u7ed3\u6784\uff08\u5982\u6539\u53d8\u914d\u4f4d\u6570\u6216\u6d3b\u6027\u4f4d\u70b9\u7684\u5206\u5e03\u4f4d\u7f6e\u7b49\uff09\u6765\u8fdb\u4e00\u6b65\u5f97\u5230\u63d0\u9ad8\u3002\u6b64\u5916\uff0c\u5728\u5b9e\u9645\u7684\u71c3\u6599\u7535\u6c60\u7b49\u88c5\u7f6e\u7684\u4f7f\u7528\u4e2d\uff0c\u9ad8\u7535\u6d41\u5bc6\u5ea6\u8fd0\u4f5c\u65f6\u50ac\u5316\u5242\u7684\u4f20\u8d28\u80fd\u529b\u6210\u4e3a\u4e86\u5f71\u54cd\u6027\u80fd\u7684\u4e3b\u5bfc\u56e0\u7d20\u3002\u7efc\u4e0a\uff0c\u5f53\u524d\u5236\u7ea6\u78b3\u57fa\u5355\u539f\u5b50\u50ac\u5316\u5242M-N\/C\u7528\u4e8eORR\u7684\u5173\u952e\u56e0\u7d20\u662f\u5176\u5b9e\u9645\u53cd\u5e94\u6d3b\u6027\u8f83\u4f4e\u53ca\u5927\u7535\u6d41\u4e0b\u7684\u4f20\u8d28\u80fd\u529b\u95ee\u9898\u3002\u4f46\u662f\uff0c\u76ee\u524d\u5f00\u53d1\u540c\u65f6\u5177\u5907\u9ad8\u6d3b\u6027\u548c\u4f18\u5f02\u7269\u8d28\u4f20\u8f93\u80fd\u529b\u7684M-N\/C\u50ac\u5316\u5242\u4ecd\u7136\u662f\u4e00\u4e2a\u5de8\u5927\u7684\u6311\u6218\u3002<\/p>\n

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

\u4e3a\u89e3\u51b3\u4e0a\u8ff0\u96be\u9898\uff0c\u8fd1\u65e5\uff0c\u6e56\u5357\u5927\u5b66\u8d39\u6167\u9f99\u6559\u6388\u3001\u53f6\u9f9a\u5170\u526f\u6559\u6388<\/b><\/strong>\u4ee5\u53ca\u4e2d\u56fd\u5730\u8d28\u5927\u5b66\u845b\u6587\u526f\u6559\u6388<\/b><\/strong>\u56e2\u961f\u91c7\u7528\u4e00\u79cd\u5f62\u8c8c\u548c\u5b54\u5de5\u7a0b\u7b56\u7565\u6765\u540c\u65f6\u8c03\u63a7Fe-N\/C\u7684\u7535\u5b50\u7ed3\u6784\u548c\u4f18\u5316\u51e0\u4f55\u7ed3\u6784\uff0c\u56e0\u6b64\u8bbe\u8ba1\u5e76\u7814\u53d1\u51fa\u4e86\u4e00\u79cd\u5177\u5907\u9ad8\u672c\u5f81\u6d3b\u6027\u548c\u4f18\u5f02\u4f20\u8d28\u80fd\u529b\u7684\u8fb9\u7f18\u7f3a\u9677FeN3<\/sub>\u4f4d\u70b9\u7684Fe-N\/C\u50ac\u5316\u5242\uff08\u547d\u540d\u4e3aeFe-N3<\/sub>\/PCF\uff09\u3002\u8be5eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u57280.1 M KOH \u4e2d\u5b9e\u73b0\u4e86\u8d85\u9ad8\u7684ORR\u6d3b\u6027\uff0c\u5982\u8d77\u59cb\u7535\u4f4d(E<\/i><\/em>onset<\/sub>)\u4e3a\u00a01.09 V,\u00a0\u534a\u6ce2\u7535\u4f4d(E<\/i><\/em>1<\/sub>\/<\/sub>2<\/sub>)\u4e3a0.934 V vs.<\/i><\/em>\u00a0RHE,\u00a0\u8fd9\u4e9b\u6027\u80fd\u6307\u6807\u5df2\u7ecf\u8fdc\u8d85\u5546\u4e1a\u5316\u7684\u8d35\u91d1\u5c5ePt\/C\u751a\u81f3\u76ee\u524d\u62a5\u9053\u7684\u6240\u6709\u78b3\u57fa\u5355\u539f\u5b50\u50ac\u5316\u5242(M-N\/C)\u3002\u6b64\u5916\uff0c\u5f53eFe-N3<\/sub>\/PCF\u7ec4\u88c5\u6210\u6c14\u4f53\u6269\u6563\u7535\u6781 (GDE)\u548c\u950c-\u7a7a\u7535\u6c60\u65f6(ZAB)\u65f6\uff0c\u5176\u5728\u5927\u7535\u6d41\u5bc6\u5ea6\u4e0b\u4e5f\u8868\u73b0\u51fa\u4f18\u5f02\u7684\u6d3b\u6027\u548c\u7a33\u5b9a\u6027\u3002\u4e00\u7cfb\u5217\u7684\u5b9e\u9a8c\u548c\u7406\u8bba\u8ba1\u7b97\u7ed3\u679c\u8868\u660e\uff1a\u8be5<\/b><\/strong>eFe-N3<\/sub>\/PCF\u7684\u9ad8\u672c\u5f81\u6d3b\u6027\u6e90\u4e8e\u5176\u4f4d\u4e8e\u8fb9\u7f18\u7684\u4f4e\u914d\u4f4d\u4e0d\u9971\u548cFe<\/b><\/strong>N<\/b><\/strong>3<\/b><\/sub><\/strong>\u4f4d\u70b9\uff0c\u800c\u5176\u5206\u7ea7\u591a\u5b54\u7ed3\u6784\u5219\u6709\u5229\u4e8e\u52a0\u5feb\u7269\u8d28\u4f20\u8f93\u4e14\u6709\u6548\u63d0\u9ad8\u539f\u5b50\u5229\u7528\u7387\uff08\u63d0\u9ad8~4\u500d\uff09<\/b><\/strong>\u3002\u8be5\u6210\u679c\u4ee5\u9898\u4e3a\u201cEdge-hosted Fe-N3<\/sub>\u00a0sites on multiscale porous carbon framework combining high intrinsic activity with efficient mass transport for oxygen reduction\u201d\u53d1\u8868\u5728\u4e86Chem<\/i><\/em>\u00a0C<\/i><\/em>atalysis<\/i><\/em>\u00a0\u4e0a\u3002\u8be5\u7814\u7a76\u4e3a\u8bbe\u8ba1\u9ad8\u6548\u5355\u539f\u5b50\u50ac\u5316\u5242\u7528\u4e8e\u65b0\u578b\u80fd\u6e90\u5b58\u50a8\u4e0e\u8f6c\u6362\u88c5\u7f6e\u4e2d\u63d0\u4f9b\u4e86\u65b0\u601d\u8def\u3002<\/p>\n

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

\u56fe1<\/b><\/strong>\u00a0<\/b><\/strong>\u50ac\u5316\u5242\u7684\u5f62\u8c8c\u548c\u5b54\u7ed3\u6784\u8868\u5f81<\/b><\/strong><\/p>\n

\"\"<\/p>\n

A) eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u7684\u7ed3\u6784\u4f18\u52bf\u793a\u610f\u56fe<\/p>\n

B) eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u7684\u626b\u63cf\u7535\u5b50\u663e\u5fae\u955c(SEM)\u56fe\uff08\u5185\u90e8\u4e3a\u5b9e\u7269\u62cd\u6444\u56fe\uff09<\/p>\n

C,\u00a0D)\u00a0eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u5728\u4f4e\u500d\u4e0b\u548c\u9ad8\u500d\u4e0b\u7684\u900f\u5c04\u7535\u5b50\u663e\u5fae\u955c(TEM)\u56fe<\/p>\n

E, F) \u50ac\u5316\u5242\u7684\u6c2e\u6c14(N2<\/sub>)\u5438\u9644\/\u8131\u9644\u66f2\u7ebf\u53ca\u76f8\u5e94\u7684\u5b54\u5f84\u5206\u5e03\u56fe<\/p>\n

G)\u50ac\u5316\u5242\u7684\u62c9\u66fc(Raman) \u5bf9\u6bd4\u56fe<\/p>\n

\u56fe2<\/b><\/strong>\u00a0<\/b><\/strong>\u50ac\u5316\u5242\u7684\u6210\u5206\u548c\u539f\u5b50\u7ed3\u6784\u5206\u6790<\/b><\/strong><\/p>\n

\"\"<\/p>\n

A) eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u7684\u50cf\u5dee\u77eb\u6b63\u900f\u5c04\u7535\u5b50\u663e\u5fae\u955c (STEM)\u56fe<\/p>\n

B) eFe-N3<\/sub>\/PCF\u50ac\u5316\u5242\u7684\u900f\u5c04\u7535\u5b50\u663e\u5fae\u955c (TEM)\u56fe\u53ca\u5143\u7d20\u5206\u5e03\u56fe<\/p>\n

C) \u50ac\u5316\u5242\u7684\u9ad8\u5206\u8fa8N1s\u00a0\u7684X\u5c04\u7ebf\u5149\u7535\u5b50\u80fd\u8c31 (XPS)\u00a0\u56fe<\/p>\n

D-F) \u50ac\u5316\u5242\u548c\u6807\u51c6\u7269\u79cd\u7684Fe\u7684K\u8fb9X\u5c04\u7ebf\u8fd1\u8fb9\u5438\u6536\u5149\u8c31 (XANES) \u56fe (D) \u548c\u5085\u91cc\u53f6\u53d8\u6362\u62d3\u5c55\u8fb9(EXAFS) \u56fe (E) \u4ee5\u53ca\u76f8\u5e94\u7684\u5c0f\u6ce2\u53d8\u6362\u56fe(F)<\/p>\n

G) \u50ac\u5316\u5242\u7684Fe\u7684K\u8fb9\u5085\u91cc\u53f6\u53d8\u6362\u62d3\u5c55\u8fb9 (EXAFS) \u56fe\u53ca\u5176\u62df\u5408\u56fe\u3002\u63d2\u56fe\u4e2d\u5206\u522b\u4e3a\u9762\u5185FeN4<\/sub>\u6a21\u578b\uff08\u4e0a\uff09\u548c\u8fb9\u7f18FeN3<\/sub>\u6a21\u578b\uff08\u4e0b\uff09\uff0c\u5176\u4e2d\u7070\u8272\u3001\u84dd\u8272\u548c\u6a59\u8272\u5c0f\u7403\u5206\u522b\u4ee3\u8868\u78b3 (C)\u3001\u6c2e (N) \u548c\u94c1 (Fe) \u539f\u5b50<\/p>\n

\u56fe<\/b><\/strong>3 RDE\u6280\u672f\u8bc4\u4ef7\u50ac\u5316\u5242\u7684ORR\u6d3b\u6027\u4ee5\u53caDFT\u5206\u6790<\/b><\/strong><\/p>\n

\"\"<\/b><\/strong><\/p>\n

A) \u50ac\u5316\u5242\u7684\u7ebf\u6027\u626b\u63cf\u4f0f\u5b89 (LSV) \u56fe (10 mV s–<\/sup>1<\/sup>,1 M KOH)<\/p>\n

B) eFe-N3<\/sub>\/PCF\u4e0e\u76ee\u524d\u62a5\u9053\u7684M-N\/C\u50ac\u5316\u5242\u7684\u6027\u80fd\u5bf9\u6bd4<\/p>\n

C) \u50ac\u5316\u5242\u7684\u534a\u6ce2\u7535\u4f4d (E<\/i><\/em>1\/2<\/sub>) \u4e0e\u52a8\u529b\u5b66\u7535\u6d41\u5bc6\u5ea6 (j<\/i><\/em>k<\/sub>, 0.8V) \u5bf9\u6bd4<\/p>\n

D) \u50ac\u5316\u5242\u7684\u4ea7H2<\/sub>O2<\/sub>\u80fd\u529b\u4e0e\u7535\u5b50\u8f6c\u79fb\u6570\u5bf9\u6bd4<\/p>\n

E) \u50ac\u5316\u5242\u7684\u53cc\u7535\u5c42\u7535\u5bb9 (C<\/i><\/em>dl<\/sub>) \u548c\u7535\u5316\u5b66\u6d3b\u6027\u9762\u79ef (ECSA) \u5bf9\u6bd4<\/p>\n

F) eFe-N3<\/sub>\/PCF\u4e0ebFe-N4<\/sub>\/PCF\u7684Fe\u539f\u5b50\u5229\u7528\u7387\u548c\u8f6c\u6362\u9891\u7387(TOF)\u5bf9\u6bd4<\/p>\n

G) eFe-N3<\/sub>\/PCF\u4e0ebFe-N4<\/sub>\/PCF\u7684\u7535\u8377\u5bc6\u5ea6\u5dee\u5206\u56fe\uff08\u84dd\u8272\u548c\u9ec4\u8272\u533a\u57df\u5206\u522b\u4ee3\u8868\u7535\u5b50\u6d88\u8017\u548c\u7d2f\u79ef\u533a\u57df\uff09<\/p>\n

H, I) 0 V (H) \u548c1.23V (I) \u4e0b\u4e24\u79cd\u6a21\u578b\u7684ORR\u81ea\u7531\u80fd\u56fe<\/p>\n

\u56fe4<\/b><\/strong>\u00a0<\/b><\/strong>\u7ec4\u88c5\u6210<\/b><\/strong>GDE\u548cZAB<\/b><\/strong>\u5668\u4ef6\u7528\u4e8e<\/b><\/strong>\u8bc4\u4ef7\u50ac\u5316\u5242\u7684ORR\u6d3b\u6027<\/b><\/strong><\/p>\n

\"\"<\/p>\n

A-C)\u00a0\u50ac\u5316\u5242\u7ec4\u88c5\u6210GDE\u7684\u7ebf\u6027\u626b\u63cf\u4f0f\u5b89 (LSV)\u56fe (10 mV s–<\/sup>1<\/sup>,\u00a01.0 M KOH) (A), 500 mA cm-2<\/sup>\u5904\u4f20\u8d28\u8fc7\u7535\u4f4d\u7684\u6bd4\u8f83(B)\u4ee5\u53ca\u963b\u6297\u5206\u6790\uff08\u5185\u90e8\u4e3a\u963b\u6297\u6a21\u62df\u56fe\uff09(C)\u00a0\u00a0<\/p>\n

D-F) \u50ac\u5316\u5242\u7ec4\u88c5\u6210ZAB\u7684\u653e\u7535\u66f2\u7ebf\u548c\u529f\u7387\u5bc6\u5ea6\u5bf9\u6bd4(D)\uff0c\u500d\u7387\u6027\u80fd(E)\u548c\u80fd\u91cf\u5bc6\u5ea6\u5bf9\u6bd4(F)<\/p>\n

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

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\u6587\u732e\u94fe\u63a5\uff1aEdge-hosted Fe-N3<\/sub>\u00a0sites on a multiscale porous carbon framework combining high intrinsic activity with efficient mass transport for oxygen reduction (Chem Catalysis, 2021, DOI:10.1016\/j.checat.2021.09.012)<\/p>\n

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