{"id":145387,"date":"2018-07-14T06:30:25","date_gmt":"2018-07-13T22:30:25","guid":{"rendered":"\/\/m.iemloyee.com\/?p=145387"},"modified":"2018-07-12T12:56:28","modified_gmt":"2018-07-12T04:56:28","slug":"angew-chem-int-ed%ef%bc%9a%e7%bc%ba%e9%99%b7%e5%b7%a5%e7%a8%8b-%e9%9d%9e%e9%87%91%e5%b1%9e%e5%9f%ba%e7%a2%b3%e6%b0%ae%e5%82%ac%e5%8c%96%e5%89%82%e7%94%a8%e4%ba%8e%e9%ab%98%e6%95%88","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=145387","title":{"rendered":"Angew. Chem. Int. Ed\uff1a\u7f3a\u9677\u5de5\u7a0b\u2014\u2014\u975e\u91d1\u5c5e\u57fa\u78b3\u6c2e\u50ac\u5316\u5242\u7528\u4e8e\u9ad8\u6548\u7535\u50ac\u5316\u56fa\u6c2e\u5408\u6210\u6c28"},"content":{"rendered":"

\u3010\u524d\u8a00\u3011<\/strong><\/p>\n

\u6c28\u662f\u4eba\u9020\u80a5\u6599\u7684\u6c2e\u6e90\uff0c\u662f\u7ef4\u6301\u4eba\u7c7b\u751f\u547d\u6700\u57fa\u672c\u7684\u5408\u6210\u5316\u5b66\u7269\u8d28\u4e4b\u4e00\u3002\u5c3d\u7ba1\u5927\u6c14\u4e2d\u7684N2<\/sub>\u662f\u53d6\u4e4b\u4e0d\u5c3d\u3001\u7528\u4e4b\u4e0d\u7aed\u7684\uff0c\u4f46N-N\u7684\u5316\u5b66\u60f0\u6027\u4f7fN2<\/sub>\u8f6c\u5316\u4e3aNH3<\/sub>\u53d8\u5f97\u56f0\u96be\u3002\u5de5\u4e1a\u4e0a\uff0cNH3<\/sub>\u7684\u5408\u6210\u901a\u5e38\u4f9d\u9760\u94c1\u57fa\u50ac\u5316\u5242\u548c\u82db\u523b\u7684\u6761\u4ef6(300\u2212400 \u00b0C\uff0cca. 250 atm)\u6765\u5b8c\u6210\u3002\u8fd9\u4e00\u8fc7\u7a0b\u5360\u4eba\u7c7b\u6d88\u8017\u7684\u5168\u90e8\u80fd\u6e90\u76841.4 %\uff0c\u540c\u65f6\u5360\u5168\u7403\u4e8c\u6c27\u5316\u78b3\u6392\u653e\u603b\u91cf\u76841.6 %\u3002\u5bfb\u6c42\u5728\u8f83\u6e29\u548c\u6761\u4ef6\u4e0b\u751f\u4ea7NH3<\/sub>\u7684\u53ef\u6301\u7eed\u6280\u672f\u4ecd\u7136\u662f\u4e00\u4e2a\u96be\u4ee5\u5b9e\u73b0\u7684\u79d1\u5b66\u548c\u6280\u672f\u76ee\u6807\u3002<\/p>\n

\u8fc7\u6e21\u91d1\u5c5e\u901a\u5e38\u88ab\u8ba4\u4e3a\u662fN2<\/sub>\u6d3b\u5316\u52a8\u529b\u5b66\u95ee\u9898\u7684\u50ac\u5316\u5242\u3002\u56e0\u6b64\uff0c\u5728\u8fc7\u53bb\u51e0\u5e74\u4e2d\uff0cNRR\u7684\u53d1\u5c55\u4e3b\u8981\u4f9d\u8d56\u4e8e\u8fc7\u6e21\u91d1\u5c5e\u57fa\u7535\u50ac\u5316\u5242\u3002\u7136\u800c\uff0c\u5728\u5b9e\u9645\u5e94\u7528\u4e2d\uff0c\u50ac\u5316\u6548\u7387\u8fd8\u6709\u5f85\u63d0\u9ad8\uff0c\u4e3b\u8981\u6e90\u4e8e\u4ee5\u4e0b\u51e0\u70b9:\u7b2c\u4e00\uff0c\u5927\u591a\u6570\u4e0e\u6c2e\u7ed3\u5408\u592a\u5f31\u7684\u8fc7\u6e21\u91d1\u5c5e\u4e0d\u80fd\u80dc\u4efbN2<\/sub>\u6d3b\u5316\uff1b\u5176\u6b21\uff0c\u8fc7\u6e21\u91d1\u5c5e\u4e2d\u7684d\u8f68\u9053\u7535\u5b50\u4e5f\u6709\u52a9\u4e8e\u4e0d\u5229\u6790\u6c22\u53cd\u5e94( HER )\u4e2d\u91d1\u5c5e- H\u952e\u7684\u5f62\u6210\uff0c\u4ece\u800c\u5bfc\u81f4\u6cd5\u62c9\u7b2c\u6548\u7387\u7684\u964d\u4f4e\u3002\u6700\u540e\uff0c\u5c3d\u7ba1\u4e00\u4e9b\u8fc7\u6e21\u91d1\u5c5e\u5728\u9002\u5f53\u7684\u7535\u4f4d\u4e0b\u4f1a\u963b\u788dHER\uff0c\u4f46\u8feb\u5207\u9700\u8981\u53ef\u884c\u7684\u66ff\u4ee3\u673a\u5236\u6765\u83b7\u5f97\u5408\u7406\u7684NRR\u6027\u80fd\u3002\u56e0\u6b64\uff0c\u7535\u50ac\u5316NRR\u7684\u8f6c\u5316\u8fdb\u5c55\u4e0d\u4ec5\u53ef\u4ee5\u4ece\u5f00\u53d1\u5168\u65b0\u7c7b\u578b\u7684\u50ac\u5316\u5242\uff0c\u800c\u4e14\u53ef\u4ee5\u901a\u8fc7\u6539\u6027\u50ac\u5316\u5242\u6765\u83b7\u5f97\u6709\u6548N2<\/sub>\u6d3b\u5316\u7684\u65b0\u673a\u5236\u3002<\/p>\n

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

\u8fd1\u65e5\uff0c\u6765\u81ea\u5fb7\u5dde\u5927\u5b66\u5965\u65af\u6c40\u5206\u6821\u7684\u4f59\u6842\u534e\u6559\u6388\u548c\u54c8\u5c14\u6ee8\u5de5\u4e1a\u5927\u5b66\u7684\u9648\u521a\u6559\u6388<\/strong>\u8054\u5408\u5728Angew. Chem. Int. Ed\u4e0a\u53d1\u8868\u6587\u7ae0\uff0c\u9898\u4e3a\uff1aDefect Engineering Metal-Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions\u3002\u7814\u7a76\u4eba\u5458\u62a5\u544a\u4e00\u79cd\u7f3a\u9677\u5de5\u7a0b\u7b56\u7565\uff0c\u4ee5\u5b9e\u73b0\u6709\u6548\u7684NRR\u6027\u80fd( NH3\u4ea7\u7387: 8.09 \u03bcg h-1<\/sup> mg-1<\/sup> cat.\uff0c\u6cd5\u62c9\u7b2c\u6548\u7387: 11.59 % )\u3002\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba(DFT)\u8ba1\u7b97\u8868\u660e\uff0c\u901a\u8fc7\u6784\u5efa\u53cc\u6838\u7a7a\u95f4\u7535\u5b50\u8f6c\u79fb\u7684\u672b\u7aef\u7ed3\u5408\u7ed3\u6784\uff0c\u4e24\u6c2e\u5206\u5b50\u53ef\u4ee5\u5316\u5b66\u5438\u9644\u5728PCN\u7684\u5de5\u7a0b\u5316\u6c2e\u7a7a\u4f4d\u4e0a\u3002\u6b64\u5916\uff0c\u5438\u9644\u7684N2<\/sub>\u7684N – N\u952e\u957f\u5ea6\u663e\u8457\u589e\u52a0\uff0c\u8fd9\u5bf9\u5e94\u4e8e\u5c06N2<\/sub>\u8fd8\u539f\u6210NH3<\/sub>\u7684\u201c\u5f3a\u6d3b\u5316\u201d\u4f53\u7cfb\u3002\u8fd9\u9879\u5de5\u4f5c\u4e5f\u5f3a\u8c03\u4e86\u7f3a\u9677\u5de5\u7a0b\u5bf9\u4e8e\u6539\u5584\u7535\u50ac\u5316\u5242\u7684\u5f31N2<\/sub>\u5438\u9644\u548c\u6d3b\u5316\u80fd\u529b\u7684\u610f\u4e49\u3002<\/p>\n

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

\u56fe 1. \u5143\u7d20\u7ed3\u6784\u8868\u5f81<\/strong><\/p>\n

\"\"<\/p>\n

(a) XRD\u56fe, (b) FTIR\u56fe, (c) TEM \u56fe (d) EPR\u56fe, (e) UV-vis DRS\uff1b<\/p>\n

(f) PCN\u548cPCN-NV4\u7684N 1s\u7684XPS\u56fe\uff1b<\/p>\n

(g) \u78b3\u6c2e\u4e2d\u6c2e\u7a7a\u4f4d\u793a\u610f\u56fe\uff1b<\/p>\n

\u56fe 2. DFT\u8ba1\u7b97<\/strong><\/p>\n

\"\"<\/p>\n

(a)\u542b\u6c2e\u7a7a\u4f4d\u7684PCN\u4e0a\u7684N2<\/sub>\u5438\u9644\u51e0\u4f55\u5f62\u72b6\uff1b<\/p>\n

(b\uff0cc)\u542b\u6c2e\u7a7a\u4f4d\u7684N2<\/sub>\u5438\u9644PCN\u7684\u7535\u8377\u5bc6\u5ea6\u5dee\uff1b\u9ec4\u8272\u548c\u84dd\u8272\u7b49\u8868\u9762\u5206\u522b\u4ee3\u8868\u7a7a\u95f4\u4e2d\u7684\u7535\u8377\u79ef\u7d2f\u548c\u8017\u5c3d\uff1b<\/p>\n

(d) NVs\u5de5\u7a0bPCN\u5728\u5e73\u8861\u7535\u4f4d\u4e0b\u7684NRR\u81ea\u7531\u80fd\u56fe\uff1b<\/p>\n

\u56fe 3. PCN-NV4\u7535\u50ac\u5316NRR\u6027\u80fd<\/strong><\/p>\n

\"\"<\/p>\n

(a) \u5728\u6bcf\u4e00\u4e2a\u7535\u4f4d\u4e0b\u7684NH3<\/sub>\u4ea7\u7387 (\u7d2b-\u7ea2) and (b) \u6cd5\u62c9\u7b2c\u6548\u7387(\u6df1\u84dd)\uff1b<\/p>\n

(c) PCN-NV4\u7684\u5faa\u73af\u6d4b\u8bd5\uff1b<\/p>\n

(d) \u5728-0.2 V versus RHE\u4e0b\u4e0d\u540c\u50ac\u5316\u5242\u7684NH3<\/sub>\u4ea7\u7387\uff1b<\/p>\n

\u56fe 4. \u4e0d\u540c\u6e29\u5ea6\u4e0bPCN-NV4\u7684NRR\u6027\u80fd<\/strong><\/p>\n

\"\"<\/p>\n

(a) \u5728\u4e0d\u540c\u6e29\u5ea6\u4e0bPCN-NV4\u7684NRR\uff1b<\/p>\n

(b) PCN-NV4\u5728\u4e0d\u540c\u6e29\u5ea6\u4e0b\u7684\u73b0\u884c\u626b\u63cf\u66f2\u7ebf\uff1b<\/p>\n

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

\u7efc\u4e0a\u6240\u8ff0\uff0c\u901a\u8fc7\u6c2e\u7a7a\u4f4d\u7f3a\u9677\u6539\u6027\u7684\u975e\u91d1\u5c5e\u57faPCN\u80fd\u4f7f\u6c28\u5728\u73af\u5883\u6761\u4ef6\u4e0b\u5408\u6210\u3002PCN – NV4\u7684NRR\u6027\u80fd\u8fbe\u52308.09 \u03bcg h-1<\/sup>mg-1<\/sup> cat.\uff0c\u6cd5\u62c9\u7b2c\u6548\u7387\u4e3a11.59 %\uff0cNH3\u4ea7\u7387\u6bd4\u672a\u542b\u6c2e\u7a7a\u4f4d\u7684\u539f\u59cbPCN\u63d0\u9ad810\u500d\u4ee5\u4e0a\u3002\u901a\u8fc7\u6839\u636e\u5148\u8fdb\u7684\u8ba1\u7b97\u6a21\u578b\u6784\u5efa\u53cc\u6838\u672b\u7aef\u7ed3\u5408\u7ed3\u6784\uff0cPCN\u4e2d\u7684\u6c2e\u7a7a\u4f4d\u4f7fN2<\/sub>\u6709\u6548\u8f6c\u5316\u4e3aNH3<\/sub>\u7684\u201c\u5f3a\u6d3b\u5316\u201d\u7cfb\u7edf\u6210\u4e3a\u53ef\u80fd\u3002\u4ee5\u4e0a\u7ed3\u679c\u53ef\u4fc3\u8fdb\u7535\u50ac\u5316\u5408\u6210NH3<\/sub>\u7684\u8fdb\u4e00\u6b65\u7814\u7a76\u548c\u53d1\u5c55\uff0c\u6307\u5bfcNRR\u591a\u79cd\u65e0\u91d1\u5c5e\u7535\u50ac\u5316\u5242\u7684\u5408\u7406\u8bbe\u8ba1\u548c\u63a2\u7d22\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1a<\/strong>Defect Engineering Metal\u2010Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions<\/a>, (Angewandte Chemie International Edition, 2018, DOI: 10.1002\/anie.201806386)<\/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

\u6295\u7a3f\u4ee5\u53ca\u5185\u5bb9\u5408\u4f5c\u53ef\u52a0\u7f16\u8f91\u5fae\u4fe1\uff1acailiaokefu\u3002<\/p>\n

\u6750\u6599\u6d4b\u8bd5\uff0c\u6570\u636e\u5206\u6790\uff0c\u4e0a<\/strong>\u6d4b\u8bd5\u8c37<\/strong><\/a>\uff01<\/strong><\/p>\n","protected":false},"excerpt":{"rendered":"

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