{"id":180118,"date":"2019-08-03T06:30:56","date_gmt":"2019-08-02T22:30:56","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=180118"},"modified":"2019-08-05T10:21:46","modified_gmt":"2019-08-05T02:21:46","slug":"%e5%8d%95%e5%8e%9f%e5%ad%90%e5%86%8d%e5%8f%91science-%e5%85%b3%e4%ba%8e%e5%8d%95%e5%8e%9f%e5%ad%90%e4%bd%a0%e7%9f%a5%e5%a4%9a%e5%b0%91%ef%bc%9f","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=180118","title":{"rendered":"\u5355\u539f\u5b50\u518d\u53d1Science\u00a0\u2014\u2014\u00a0\u5173\u4e8e\u5355\u539f\u5b50\u4f60\u77e5\u591a\u5c11\uff1f"},"content":{"rendered":"

\u968f\u7740\u7eb3\u7c73\u50ac\u5316\u7684\u53d1\u5c55\u548c\u8868\u5f81\u6280\u672f\u7684\u8fdb\u6b65\uff0c\u79d1\u7814\u5de5\u4f5c\u8005\u53d1\u73b0\u8868\u9762\u4e0d\u9971\u548c\u914d\u4f4d\u539f\u5b50\u5f80\u5f80\u662f\u50ac\u5316\u7684\u6d3b\u6027\u4f4d\u70b9\uff0c\u6240\u4ee5\u901a\u8fc7\u63a7\u5236\u7eb3\u7c73\u6676\u7684\u5c3a\u5bf8\u3001\u5f62\u8c8c\u3001\u6676\u9762\u53bb\u8c03\u63a7\u50ac\u5316\u5242\u8868\u9762\u539f\u5b50\u7684\u5206\u5e03\u548c\u7ed3\u6784\u4ee5\u63d0\u9ad8\u50ac\u5316\u6027\u80fd\u3002\u5f53\u7eb3\u7c73\u6676\u5c3a\u5bf8\u964d\u4f4e\u5230\u539f\u5b50\u56e2\u7c07\u3001\u5355\u539f\u5b50\u65f6\uff0c\u5176\u80fd\u7ea7\u7ed3\u6784\u548c\u7535\u5b50\u7ed3\u6784\u4f1a\u53d1\u751f\u6839\u672c\u6027\u7684\u53d8\u5316\uff0c\u6b63\u662f\u7531\u4e8e\u8fd9\u79cd\u72ec\u7279\u7684\u7ed3\u6784\u7279\u70b9\uff0c\u4f7f\u5f97\u5355\u539f\u5b50\u50ac\u5316\u5242\u5f80\u5f80\u8868\u73b0\u51fa\u4e0d\u540c\u4e8e\u4f20\u7edf\u7eb3\u7c73\u50ac\u5316\u5242\u7684\u6d3b\u6027\u3001\u9009\u62e9\u6027\u548c\u7a33\u5b9a\u6027\u3002\u5355\u539f\u5b50\u6750\u6599\u4e0d\u4ec5\u4e3a\u4ece\u5206\u5b50\u5c42\u6b21\u8ba4\u8bc6\u50ac\u5316\u53cd\u5e94\u7684\u673a\u7406\u63d0\u4f9b\u4e86\u7406\u60f3\u7684\u6a21\u578b\u548c\u7814\u7a76\u5e73\u53f0\uff0c\u800c\u4e14\u6709\u671b\u6210\u4e3a\u5177\u6709\u5de5\u4e1a\u50ac\u5316\u5e94\u7528\u6f5c\u529b\u7684\u65b0\u578b\u50ac\u5316\u5242\u3002<\/p>\n

2019\u5e746\u670814\u65e5\uff0cScience\u5728\u7ebf\u51fa\u7248\u4e86\u6d1b\u6851\u7406\u5de5\u5b66\u9662\u548c\u56fd\u7acb\u53f0\u6e7e\u5927\u5b66\u8054\u5408\u53d1\u8868\u7684Fe(\u2162)\u5355\u539f\u5b50\u56fa\u5b9a\u4e8e\u63ba\u6742N\u7684\u78b3\u8f7d\u4f53\u4e0a\uff0c\u7528\u4e8e\u9ad8\u6548CO2<\/sub>\u8fd8\u539f\uff0c\u4e3a\u5355\u539f\u5b50\u50ac\u5316\u7684\u8bbe\u8ba1\u3001\u673a\u7406\u63d0\u4f9b\u4e86\u65b0\u7684\u601d\u8def\u548c\u65b9\u5411\u3002\u672c\u6587\u7ed3\u5408\u8fd1\u671f\u53d1\u8868\u7684\u9ad8\u8d28\u91cfSCI\u8bba\u6587\u5c31\u5355\u539f\u5b50\u50ac\u5316\u7684\u5e94\u7528\u3001\u5236\u5907\u548c\u8868\u5f81\u4f5c\u7b80\u5355\u603b\u7ed3\uff0c\u4ee5\u4f9b\u53c2\u8003\uff08\u672c\u6587\u4ec5\u8868\u8fbe\u4f5c\u8005\u4e2a\u4eba\u89c2\u70b9\uff09\u3002<\/p>\n

\u4e00\u3001\u6700\u65b0\u6210\u679c\u7b80\u4ecb<\/strong><\/p>\n

1\u3001Science<\/b><\/strong>: Atomically dispersed Fe3+<\/sup>\u00a0sites catalyze efficient CO2\u00a0<\/sub>electroreduction to CO<\/p>\n

\u6d1b\u6851\u7406\u5de5\u5b66\u9662\u548c\u56fd\u7acb\u53f0\u6e7e\u5927\u5b66\u8054\u5408\u62a5\u544a\u4e86\u4e00\u79cd\u7531\u5206\u6563\u7684\u5355\u539f\u5b50Fe\u6d3b\u6027\u4f4d\u70b9\u7ec4\u6210\u7684\u50ac\u5316\u5242\uff08\u5982\u56fe1\u6240\u793a\uff09\uff0c\u8fd9\u79cd\u50ac\u5316\u5242\u5728\u4f4e\u81f380\u6beb\u4f0f\u7684\u8fc7\u7535\u52bf\u4e0b\u4ea7\u751f\u4e00\u6c27\u5316\u78b3\u3002\u5728340\u6beb\u4f0f\u7684\u8fc7\u7535\u52bf\u4e0b\uff0c\u5206\u7535\u6d41\u5bc6\u5ea6\u8fbe\u523094\u6beb\u5b89\u57f9\u6bcf\u5e73\u65b9\u5398\u7c73\u3002Operando X\u5c04\u7ebf\u5438\u6536\u5149\u8c31\u663e\u793a\u5176\u6d3b\u6027\u4f4d\u70b9\u662f\u79bb\u6563\u7684\u3001\u4e0eN\u63ba\u6742\u7684\u78b3\u8f7d\u4f53\u914d\u4f4d\u7684Fe3+<\/sup>\u79bb\u5b50\uff0c\u5e76\u5728\u7535\u50ac\u5316\u8fc7\u7a0b\u4e2d\u4fdd\u6301\u5176+3\u6c27\u5316\u72b6\u6001\u3002\u7535\u5316\u5b66\u6570\u636e\u8868\u660e\uff0cFe3+<\/sup>\u4f4d\u70b9\u6bd4\u4f20\u7edfFe2+<\/sup>\u4f4d\u70b9\u5177\u6709\u66f4\u5feb\u7684CO2<\/sub>\u5438\u9644\u901f\u5ea6\u00a0[1]<\/sup>\u3002<\/p>\n

\u56fe1 Fe(3+)\u5355\u539f\u5b50\u7684\u7269\u6027\u8868\u5f81<\/p>\n

\"\" \u00a0\u00a0\u00a0<\/p>\n

\u4e8c\u3001\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u5e94\u7528<\/strong><\/p>\n

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1\u3001CO2<\/sub>\u8fd8\u539f<\/strong><\/p>\n

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\u7b2c\u4e00\u90e8\u5206\u6240\u8ff0\u7684Fe(3+)\u5355\u539f\u5b50\u50ac\u5316\u5242\u5728CO2<\/sub>\u8fd8\u539f\u4e2d\u4fbf\u5177\u6709\u8f83\u4f4e\u7684\u8fc7\u7535\u52bf [1]<\/sup>\u30022019\u5e742\u6708\uff0c\u4e2d\u56fd\u79d1\u5b66\u6280\u672f\u5927\u5b66\u5434\u5b87\u6069\u8bfe\u9898\u7ec4\u5728Joule\u53d1\u8868\u4e86\u4e00\u79cd\u7531\u5927\u5757\u91d1\u5c5e\u51fa\u53d1\u5408\u6210\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u65b9\u6cd5\u3002\u4ed6\u4eec\u8bc1\u660e\u4e86\u5728N\u63ba\u6742\u78b3\u548c\u5927\u5757\u954d\u91d1\u5c5e\u4e4b\u95f4\u7684\u56fa\u6001\u6269\u6563\u53ef\u7528\u4e8e\u5408\u6210\u5206\u7ea7\u3001\u81ea\u652f\u6491\u3001\u539f\u5b50\u7ea7\u7684Ni\u57fa\u50ac\u5316\u5242\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\u8be5\u65b9\u6cd5\u53ef\u91cf\u4ea7\uff0c\u4ee5\u6ee1\u8db3\u5de5\u4e1a\u9700\u6c42\u3002\u6240\u83b7\u5f97\u7684\u6837\u54c1\u53ef\u76f4\u63a5\u7528\u4f5c\u65e0\u7c98\u7ed3\u5242\u7535\u6781\uff0c\u7528\u4e8eCO2<\/sub>\u7535\u89e3\u8fd8\u539f\uff0c\u5177\u6709\u9ad8\u6c34\u51c6\u7684\u6027\u80fd\u00a0[2]<\/sup>\u30022018\u5e743\u6708\uff0c\u674e\u4e9a\u680b\u7b49\u62a5\u9053\u4e86\u4e00\u79cd\u9ad8\u6d3b\u6027\u3001\u9ad8\u9009\u62e9\u6027\u7684\u5355\u539f\u5b50Co-N5<\/sub>\u50ac\u5316\u5242\u3002\u8be5\u50ac\u5316\u5242\u5177\u6709\u539f\u5b50\u7ea7\u5206\u6563\u7684Co\u6d3b\u6027\u4e2d\u5fc3\u56fa\u5b9a\u4e8e\u805a\u5408\u7269\u884d\u751f\u7684\u4e2d\u7a7aN\u63ba\u6742\u591a\u5b54\u78b3\u7403\u4e0a\uff0c\u5982\u56fe2\u6240\u793a\u3002\u7535\u5316\u5b66\u6d4b\u8bd5\u7ed3\u679c\u8868\u660e\uff0c\u8fd9\u79cd\u5355\u539f\u5b50Co\u50ac\u5316\u5242\u5728-0.73\u548c-0.79V\u4e0b\u7684CO\u6cd5\u62c9\u7b2c\u6548\u7387\u5206\u522b\u4e3a99.2%\u548c99.4%\uff0c\u76f8\u6bd4\u4e8e\u915e\u83c1\u94b4\u63d0\u5347\u4e8615.5\u500d\u3002\u5728-0.57\u5230-0.88 V\u7684\u8303\u56f4\u5185\uff0c\u8be5\u50ac\u5316\u5242\u8fd8\u8868\u73b0\u51fa\u8f83\u9ad8\u7684CO\u6cd5\u62c9\u7b2c\u6548\u7387\uff08>90%\uff09\u3002\u7ed3\u5408\u5b9e\u9a8c\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\uff0c\u4f5c\u8005\u63a8\u65ad\u5355\u539f\u5b50Co-N5<\/sub>\u4f4d\u70b9\u540c\u65f6\u662f\u4e8c\u6c27\u5316\u78b3\u6d3b\u5316\u53ca\u53cd\u5e94\u4e2d\u95f4\u4f53COOH*\u7684\u4e3b\u8981\u6d3b\u6027\u4e2d\u5fc3 [3]<\/sup>\u3002<\/p>\n

\u56fe2 \u5355\u539f\u5b50Co-N5<\/sub>\u50ac\u5316\u5242\u7684\u5408\u6210\u4e0e\u8868\u5f81<\/p>\n

\"\"<\/p>\n

2. ORR<\/strong><\/p>\n

\u53d1\u751f\u5728\u7535\u5316\u5b66\u80fd\u5668\u4ef6\u9634\u6781\u4e0a\u7684ORR\u901a\u8fc7\u4e24\u7535\u5b50\uff082e–<\/sup>\uff09\u6216\u56db\u7535\u5b50\uff084e–<\/sup>\uff09\u9014\u5f84\u8fdb\u884c\u3002\u7531\u4e8e\u56db\u7535\u5b50\u8def\u5f84\u5177\u6709\u8f83\u9ad8\u7684\u80fd\u91cf\u8f6c\u6362\u6548\u7387\uff0c\u56e0\u6b64\u5b83\u53ef\u4ee5\u5c06\u6c27\u6c14\u76f4\u63a5\u8fd8\u539f\u4e3a\u6c34\uff0c\u56e0\u800c\u5728\u71c3\u6599\u7535\u6c60\u548c\u91d1\u5c5e-\u7a7a\u6c14\u7535\u6c60\u4e2d\u662f\u9996\u9009\u7684\u8def\u5f84\u3002\u5355\u539f\u5b50\u50ac\u5316\u5242\u5df2\u88ab\u62a5\u9053\u53ef\u4f5c\u4e3a\u4e00\u79cd\u9ad8\u6548\u7684ORR\u50ac\u5316\u5242\u3002<\/p>\n

2019\u5e742\u6708\uff0c\u52a0\u62ff\u5927\u97e6\u4ed5\u6566\u5927\u5b66\u5b59\u5b66\u826f\u6559\u6388\u7b49\u62a5\u9053\u4e86\u4e00\u79cd\u7ade\u4e89\u6027\u7edc\u5408\u7b56\u7565\u7528\u4e8e\u5408\u6210Co-Zn\u5355\u539f\u5b50\u5bf9\u7528\u4e8eORR\u53ca\u950c\u7a7a\u7535\u6c60\u3002\u8fd9\u79cdCo-Zn\u5355\u539f\u5b50\u5bf9\u914d\u4f4d\u4e8eN\u63ba\u6742\u78b3\u8f7d\u4f53\u4e0a\uff0c\u663e\u8457\u5ef6\u957f\u4e86O-O\u952e\u7684\u957f\u5ea6\uff08\u4ece1.23\u57c3\u52301.42\u57c3\uff09\uff0c\u4ece\u800c\u4fc3\u8fdb\u4e86O-O\u952e\u7684\u5206\u88c2\u3002\u8fd9\u79cd\u50ac\u5316\u5242\u5728\u78b1\u6027\u548c\u9178\u6027\u6761\u4ef6\u4e0b\u5747\u8868\u73b0\u51fa\u51fa\u8272\u7684ORR\u6027\u80fd\u3002\u539f\u4f4dXANES\u5206\u6790\u8868\u660e\uff0c\u5728ORR\u8fc7\u7a0b\u4e2d\uff0c\u5355\u539f\u5b50Co\u662f\u6d3b\u6027\u4e2d\u5fc3 [4]<\/sup>\u3002<\/p>\n

2019\u5e743\u6708\uff0c\u5316\u5b66\u6240\u4e07\u7acb\u4fca\u53d1\u8868\u4e86\u4e00\u79cd\u901a\u7528\u7b56\u7565\u7528\u4e8e\u5236\u5907\u9ad8\u8f7d\u91cf\u7684\u91d1\u5c5e-N\u5355\u539f\u5b50\u50ac\u5316\u5242\uff0c\u8f7d\u91cf\u9ad8\u8fbe\u00a012.1\u2009wt%\u3002\u5176\u4e2d\uff0cFe\u5355\u539f\u5b50\u50ac\u5316\u5242\u5177\u6709\u5f88\u597d\u7684ORR\u6d3b\u6027\u3002\u7ed3\u679c\u8868\u660e\uff0c\u5c06\u8461\u8404\u7cd6\u4e0eFe\u79bb\u5b50\u87af\u5408\u3001\u5927\u91cf\u7684\u542b\u6c27\u529f\u80fd\u65cf\u53ca\u5927\u7684\u6bd4\u8868\u9762\u79ef\u7684\u652f\u6491\u4ee5\u53ca\u542bN\u529f\u80fd\u65cf\u7b49\u7686\u662f\u5408\u6210\u9ad8\u8f7d\u91cfFe\u5355\u539f\u5b50\u590d\u5408\u7269\u7684\u5173\u952e\u6761\u4ef6\u3002\u5f97\u76ca\u4e8e\u9ad8\u8f7d\u91cf\u7684Fe-N\u5355\u539f\u5b50\u6240\u66b4\u9732\u7684\u6d3b\u6027\u4f4d\u70b9\uff0c\u8fd9\u79cdFe-N\u5355\u539f\u5b50\u50ac\u5316\u5242\u8868\u73b0\u51fa\u4f18\u4e8ePt-C\u7535\u6781\u7684ORR\u50ac\u5316\u6027\u80fd\uff0c\u5982\u56fe3\u6240\u793a [5]<\/sup>\u3002<\/p>\n

2019\u5e744\u6708\uff0cNature Catalysis\u53d1\u8868\u4e86\u4e2d\u56fd\u79d1\u5b66\u6280\u672f\u5927\u5b66\u5434\u5b87\u6069\u8bfe\u9898\u7ec4\u7684Ru\u5355\u539f\u5b50\u50ac\u5316\u5242\uff0c\u7528\u4e8e\u9ad8\u6548\u7684OER\u6d3b\u6027\u30022019\u5e745\u6708\uff0c\u9655\u897f\u5e08\u8303\u5927\u5b66\u5728Nature Commun.\u5728\u7ebf\u53d1\u8868\u4e86\u4e00\u79cd\u5355\u539f\u5b50W\u50ac\u5316\u5242\uff0c\u4e5f\u5177\u6709\u6770\u51fa\u7684OER\u6027\u80fd\u3002<\/p>\n

\u56fe3 \u5355\u539f\u5b50Fe-N\u50ac\u5316\u5242\u7684ORR\u6027\u80fd\u3002<\/p>\n

\"\"<\/p>\n

3.HER<\/strong><\/p>\n

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4.\u4fc3\u8fdb\u591a\u786b\u5316\u9502\u5411\u786b\u5316\u9502\u7684\u8f6c\u6362<\/strong><\/p>\n

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2019\u5e742\u6708\uff0c\u4e2d\u56fd\u79d1\u5b66\u6280\u672f\u5927\u5b66\u5b63\u6052\u661f\u7b49\u62a5\u9053\u4e86\u4e00\u79cd\u5355\u539f\u5b50Co\u50ac\u5316\u5242\uff08\u5982\u56fe4\u6240\u793a\uff09\uff0c\u7528\u4e8e\u4fc3\u8fdb\u591a\u786b\u5316\u9502\u5411\u786b\u5316\u9502\u7684\u8f6c\u6362\u3002\u5229\u7528Operando X\u5c04\u7ebf\u5438\u6536\u5149\u8c31\u548c\u7b2c\u4e00\u539f\u7406\u8ba1\u7b97\u76f8\u7ed3\u5408\uff0c\u4ed6\u4eec\u53d1\u73b0\u5355\u539f\u5b50Co-N-C\u914d\u4f4d\u4e2d\u5fc3\u662f\u4e00\u4e2a\u53cc\u529f\u80fd\u7535\u50ac\u5316\u5242\uff0c\u53ef\u4ee5\u5206\u522b\u4fc3\u8fdb\u653e\u7535\u548c\u5145\u7535\u8fc7\u7a0b\u4e2dLi2<\/sub>S\u7684\u5f62\u6210\u548c\u5206\u89e3\u3002\u4ee5\u542bCo\u5355\u539f\u5b50\u7684N\u63ba\u6742\u77f3\u58a8\u70ef\u4e3a\u57fa\u5e95\uff0c\u8d1f\u8f7d90%\u9ad8\u8f7d\u91cf\u7684S\u7528\u4e8eLi-S\u7535\u6c60\uff0c\u5177\u67091210mAh\/g\u7684\u53ef\u9006\u5bb9\u91cf\u53ca5.1mAh\/cm2<\/sup>\u7684\u9762\u5bb9\u91cf [8]<\/sup>\u3002<\/p>\n

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1.\u7a7a\u4f4d\u7f3a\u9677\u951a\u5b9a\u7b56\u7565<\/strong><\/p>\n

\u4e3a\u4e86\u9650\u5236\u91d1\u5c5e\u539f\u5b50\u5728\u57fa\u5e95\u4e0a\u7684\u8fc1\u79fb\uff0c\u5bf9\u57fa\u5e95\u4e0a\u7684\u7f3a\u9677\u8fdb\u884c\u63a7\u5236\u662f\u4e00\u79cd\u6709\u6548\u7684\u65b9\u6cd5\u3002\u7f3a\u9677\u7684\u5b58\u5728\u4f1a\u6539\u53d8\u5468\u56f4\u7684\u7535\u5b50\u7ed3\u6784\u548c\u914d\u4f4d\u73af\u5883\uff0c\u5bfc\u81f4\u51fa\u73b0\u7a7a\u4f4d\u548c\u4e0d\u9971\u548c\u7684\u914d\u4f4d\u4f4d\u70b9\u3002\u57fa\u5e95\u4e0a\u7684\u8fd9\u4e9b\u7f3a\u9677\u53ef\u4ee5\u4f5c\u4e3a\u201c\u9677\u9631\u201d\uff0c\u5728\u540e\u5904\u7406\u8fc7\u7a0b\u4e2d\u6355\u83b7\u91d1\u5c5e\u524d\u9a71\u4f53\u53ca\u951a\u5b9a\u91d1\u5c5e\u539f\u5b50\u3002\u9633\u79bb\u5b50\u7a7a\u4f4d\u4f5c\u4e3a\u4e00\u7c7b\u5178\u578b\u7684\u7f3a\u9677\uff0c\u8fd1\u5e74\u6765\u5df2\u88ab\u5e7f\u6cdb\u7528\u4e8e\u5408\u6210\u5355\u539f\u5b50\u50ac\u5316\u5242\u3002\u5728\u5e94\u7528\u7f3a\u9677\u5de5\u7a0b\u7b56\u7565\u5408\u6210\u5355\u539f\u5b50\u65f6\uff0c\u9996\u5148\u8981\u4f18\u5316\u7f3a\u9677\u5de5\u7a0b\u7684\u5f62\u6210\u6761\u4ef6\uff0c\u4ee5\u786e\u4fdd\u5f62\u6210\u5747\u5300\u7684\u7f3a\u9677\u4e2d\u5fc3\u4f5c\u4e3a\u951a\u5b9a\u70b9\uff0c\u4f7f\u5355\u4e2a\u539f\u5b50\u5747\u5300\u4e14\u7a33\u5b9a\u3002\u6b64\u5916\uff0c\u8fd8\u5e94\u660e\u786e\u7f3a\u9677\u7c7b\u578b\uff0c\u8fd9\u6837\u6709\u5229\u4e8e\u9009\u62e9\u5408\u9002\u7684\u91d1\u5c5e\u79cd\u7c7b\u4f5c\u4e3a\u524d\u8eaf\u4f53\uff0c\u5e76\u91c7\u53d6\u76f8\u5e94\u63aa\u65bd\u907f\u514d\u540e\u5904\u7406\u8fc7\u7a0b\u4e2d\u7f3a\u9677\u7684\u6d88\u5931\u548c\u8f6c\u5316\u3002<\/p>\n

\u4f8b\u5982\uff0cTsang\u7b49\u63ed\u793a\u4e86\u786b\u7a7a\u4f4d\u5728\u5f62\u6210\u6297\u70e7\u7ed3\u7684\u5355\u5206\u6563\u91d1\u5c5e\u539f\u5b50\u4e2d\u7684\u91cd\u8981\u4f5c\u7528\u3002\u4ed6\u4eec\u901a\u8fc7\u9502\u63d2\u5c42\u548c\u5316\u5b66\u5265\u8131\u4f5c\u7528\u5408\u6210\u4e86\u57fa\u9762\u4e0a\u786b\u7a7a\u4f4d\u4e30\u5bcc\u7684MoS2<\/sub>\u5355\u5206\u5b50\u5c42\uff0c\u8fd9\u4e9b\u542b\u786b\u7f3a\u9677\u7684MoS2<\/sub>\u5206\u5b50\u5c42\u53ef\u4ee5\u901a\u8fc7\u586b\u5145S\u7a7a\u4f4d\u6765\u6355\u83b7\u5e76\u7ed3\u5408\u5177\u6709\u9ad8\u4eb2\u548c\u529b\u7684\u786b\u8132\u57faCo\u914d\u5408\u7269\uff0c\u4ece\u800c\u83b7\u5f97\u5355\u5206\u6563\u7684Co\u539f\u5b50\u5206\u6563\u4e8eMoS2<\/sub>\u8584\u5c42\u4e0a\uff08\u5982\u56fe5\u6240\u793a\uff09\u3002\u5b9e\u9a8c\u548cDFT\u8ba1\u7b97\u8868\u660e\uff0cCo\u539f\u5b50\u4e0e\u5355\u5c42MoS2<\/sub>\u5177\u6709\u8f83\u5f3a\u7684\u5171\u4ef7\u7ed3\u5408\u80fd\u529b\uff0c\u5e76\u4e14\u5728S\u7a7a\u4f4d\u7684\u4f5c\u7528\u4e0b\u5f62\u6210\u4e86Co-S-Mo\u754c\u9762\uff0c\u56e0\u6b64\u5177\u6709\u610f\u60f3\u4e0d\u5230\u7684\u6d3b\u6027\u548c\u826f\u597d\u7684\u7a33\u5b9a\u6027 [10]<\/sup>\u3002\u78b3\u57fa\u6750\u6599\u4e2d\u4e5f\u7ecf\u5e38\u51fa\u73b0\u7a7a\u4f4d\u3002\u901a\u8fc7\u91d1\u5c5e\u539f\u5b50\u548c\u78b3\u539f\u5b50\u4e4b\u95f4\u7684\u7535\u5b50\u8f6c\u79fb\uff0c\u7a7a\u4f4d\u53ef\u4ee5\u4f5c\u4e3a\u56fa\u5b9a\u91d1\u5c5e\u539f\u5b50\u7684\u4f4d\u7f6e\u3002\u4f8b\u5982\uff0cNi\u539f\u5b50\u4e0e\u5468\u56f4C\u539f\u5b50\u4e4b\u95f4\u7684\u7535\u8377\u8f6c\u79fb\u662f\u5355\u539f\u5b50Ni\u5728\u9178\u6027\u6eb6\u6db2\u4e2d\u9ad8\u5ea6\u7a33\u5b9a\u7684\u91cd\u8981\u539f\u56e0 [11]<\/sup>\u3002<\/p>\n

\u56fe5 \u5206\u6563\u4e8e\u5355\u5c42MoS2<\/sub>\u57fa\u5e95\u7684\u4ee5S\u7a7a\u4f4d\u7a33\u5b9a\u7684Co\u5355\u539f\u5b50\u590d\u5408\u7269\u7684\u7269\u6027\u8868\u5f81\u3002<\/p>\n

\"\"<\/p>\n

2. \u7a7a\u95f4\u9650\u57df\u7b56\u7565<\/strong><\/p>\n

\u5c06\u5355\u4e2a\u91d1\u5c5e\u539f\u5b50\u7a7a\u95f4\u9650\u5236\u5728\u5206\u5b50\u5c3a\u5ea6\u7684\u7b3c\u4e2d\u4ee5\u9632\u6b62\u5176\u8fc1\u79fb\uff0c\u5df2\u6210\u4e3a\u4e00\u79cd\u6709\u6548\u7684\u5408\u6210\u5355\u539f\u5b50\u590d\u5408\u7269\u7684\u65b9\u6cd5\u3002\u901a\u5e38\uff0c\u8fd9\u79cd\u7a7a\u95f4\u9650\u5236\u7b56\u7565\u5305\u62ec\u4e24\u4e2a\u6b65\u9aa4\uff1a\uff081\uff09\u501f\u52a9\u5206\u5b50\u7b5b\u3001MOF\u548c\u5171\u4ef7\u6709\u673a\u6846\u67b6\u7b49\u591a\u5b54\u6750\u6599\u5206\u79bb\u548c\u5c01\u88c5\u5408\u9002\u7684\u5355\u6838\u91d1\u5c5e\u524d\u8eaf\u4f53\uff0c\u5b9e\u73b0\u91d1\u5c5e\u7269\u79cd\u7684\u9ad8\u7a7a\u95f4\u5206\u5e03\u548c\u539f\u5b50\u5206\u6563\u3002\uff082\uff09\u901a\u8fc7\u540e\u5904\u7406\u53bb\u9664\u524d\u4f53\u7684\u914d\u4f53\uff0c\u5f62\u6210\u5355\u4e00\u7684\u91d1\u5c5e\u539f\u5b50\uff0c\u5e76\u901a\u8fc7\u8f7d\u4f53\u9aa8\u67b6\u7a33\u5b9a\u4e0b\u6765\u3002<\/p>\n

\u4f8b\u5982\uff0c\u674e\u4e9a\u680b\u548c\u738b\u5b9a\u80dc\u7b49\u901a\u8fc7MOF\u4e2d\u5747\u5300\u8fde\u901a\u7684\u5b54\u4f5c\u4e3a\u7b3c\uff0c\u5b9e\u73b0\u4e86\u91d1\u5c5e\u79cd\u7c7b\u7684\u7a7a\u95f4\u5206\u79bb\u548c\u9650\u5236\uff0c\u4ece\u800c\u5236\u5907\u51fa\u5355\u5206\u6563\u91d1\u5c5e\u539f\u5b50\u3002\u5982\u56fe6\u6240\u793a\uff0c\u901a\u8fc7\u4f7f\u7528ZIF-8\u7684\u5206\u5b50\u5c3a\u5ea6\u7a7a\u8154\u4f5c\u4e3a\u5bbf\u4e3b\uff0c\u4e00\u4e2a\u94c1\uff08III\uff09\u4e59\u9170\u4e19\u916e\u5206\u5b50\uff08Fe(Acac)3<\/sub>\uff09\u53ef\u4ee5\u88ab\u4e00\u4e2a\u7a7a\u8154\u5206\u79bb\u548c\u5c01\u88c5\uff0c\u5e76\u4e14\u4e0d\u4f1a\u88ab\u91ca\u653e\uff0c\u56e0\u4e3aFe(Acac)3<\/sub>\u7684\u5206\u5b50\u76f4\u5f84\uff08\u7ea69.7 \u57c3\uff09\u4f4d\u4e8eZIF-8\u7684\u5b54\uff08\u7ea63.4\u57c3\uff09\u548c\u7b3c\u5f84\uff08\u7ea611.6\u57c3\uff09\u4e4b\u95f4\u3002\u56e0\u6b64\uff0c\u7ecf\u8fc7\u70ed\u5206\u89e3\u540e\uff0c\u5f62\u6210\u4e86\u7531\u6c2e\u5143\u7d20\u56fa\u5b9a\u7684\u7a33\u5b9a\u7684\u5355\u5206\u6563\u94c1\u539f\u5b50\u00a0[12]<\/sup>\u3002<\/p>\n

\u56fe6 \u5229\u7528MOF\u9650\u57df\u5f62\u6210\u7684Fe\u5355\u5b50\u7684\u5408\u6210\u53ca\u8868\u5f81\u3002<\/p>\n

\"\" \u00a0\u00a0<\/p>\n

3.\u914d\u4f4d\u8bbe\u8ba1\u7b56\u7565<\/strong><\/p>\n

\u5408\u7406\u8bbe\u8ba1\u914d\u4f4d\u70b9\u4f5c\u4e3a\u201c\u722a\u201d\uff0c\u4ee5\u5438\u9644\u548c\u7ed3\u5408\u91d1\u5c5e\u524d\u9a71\u4f53\u6216\u91d1\u5c5e\u539f\u5b50\uff0c\u9632\u6b62\u5176\u8fc1\u79fb\u548c\u51dd\u805a\uff0c\u4ece\u800c\u5408\u6210\u4e86\u5355\u539f\u5b50\u50ac\u5316\u5242\u3002\u57fa\u4e8e\u91d1\u5c5e\u539f\u5b50\u548c\u914d\u4f4d\u539f\u5b50N\u3001O\u548cS\u4e4b\u95f4\u7684\u5f3a\u7684\u76f8\u4e92\u4f5c\u7528\uff0c\u7528\u8fd9\u4e9b\u914d\u4f4d\u539f\u5b50\u4f5c\u4e3a\u951a\u5b9a\u4f4d\u70b9\u6765\u6784\u9020\u652f\u6491\u7269\uff0c\u4ee5\u83b7\u5f97\u5355\u5206\u6563\u7684\u539f\u5b50\u7ea7\u50ac\u5316\u5242\u3002<\/p>\n

\u4f8b\u5982\uff0c2019\u5e743\u6708\uff0c\u6d59\u6c5f\u5927\u5b66\u548c\u65af\u987f\u5de5\u4e1a\u5927\u5b66\u7684\u5408\u4f5c\u8bba\u6587Atomically dispersed nickel\u2013nitrogen\u2013sulfur species anchored on porous carbon nanosheets for efficient water oxidation\u62a5\u5bfc\u4e86\u4e00\u79cd\u539f\u5b50\u7ea7\u5206\u6563\u7684S\u3001N\u914d\u4f4d\u7684Ni\u5355\u539f\u5b50OER\u50ac\u5316\u5242\u3002\u8fd9\u79cdNi\u5355\u539f\u5b50\u4e0e\u591a\u5b54\u78b3\u7eb3\u7c73\u7247\u4e2d\u7684\u6c2e\u548c\u786b\u914d\u4f4d\uff0c\u4ece\u800c\u7a33\u5b9a\u5206\u6563\u4e8eN\u63ba\u6742C\u57fa\u5e95\u4e0a\u3002\u4f5c\u4e3a\u4e00\u79cd\u7535\u50ac\u5316\u5242\uff0c\u572810 mA\/cm2<\/sup>\u6761\u4ef6\u4e0b\u5177\u67091.51V\u7684\u8f83\u5c0f\u8fc7\u7535\u52bf\u548c45 mV\/dec\u7684\u5c0f\u5854\u83f2\u5c14\u659c\u7387\uff0c\u5982\u56fe7\u6240\u793a\u3002\u8fd9\u79cd\u7535\u50ac\u5316\u5242\u662f\u6240\u6709\u62a5\u9053\u8fc7\u7684\u8fc7\u6e21\u91d1\u5c5e\u548c\u6742\u539f\u5b50\u63ba\u6742\u7684\u78b3\u7535\u50ac\u5316\u5242\u4e2d\u6700\u597d\u7684\uff0c\u751a\u81f3\u4f18\u4e8eIr\/C\u50ac\u5316\u5242\u00a0[13]<\/sup>\u3002<\/p>\n

\u56fe7 \u6c2e\u548c\u786b\u914d\u4f4d\u7684Ni\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684OER\u6027\u80fd\u3002<\/p>\n

\"\"<\/p>\n

\u56db\u3001\u5355\u539f\u5b50\u50ac\u5316\u5242\u8868\u5f81\u65b9\u6cd5<\/strong><\/p>\n

\u5bf9\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u8868\u5f81\uff0c\u6700\u76f4\u89c2\u7684\u65b9\u6cd5\u5c31\u662f\u7403\u5dee\u77eb\u6b63\u7535\u955c\uff08Sub-angstrom-resolution aberration-corrected scanning transmission electron microscopy, AC-STEM)\u6280\u672f\u76f4\u63a5\u5bf9\u5206\u6563\u4e8e\u9ad8\u6bd4\u8868\u9762\u79ef\u8f7d\u4f53\u8868\u9762\u7684\u5355\u4e2a\u539f\u5b50\u8fdb\u884c\u6210\u50cf\u3002\u800cX-\u5c04\u7ebf\u8fd1\u8fb9\u5438\u6536\u8c31\uff08X-ray absorption near edge spectroscopy, XANES\uff09\u548c\u6269\u5c55\u8fb9X-\u5c04\u7ebf\u5438\u6536\u7cbe\u7ec6\u7ed3\u6784\u8c31\uff08X-ray absorption fine structure spectroscopy, EXAFS) \u4e5f\u53ef\u4ee5\u63d0\u4f9b\u5173\u4e8e\u5355\u539f\u5b50\u7684\u6c27\u5316\u6001\u3001\u914d\u4f4d\u60c5\u51b5\u7b49\u4fe1\u606f\u3002<\/p>\n

1.\u7535\u955c\u6280\u672f<\/strong><\/p>\n

\u7535\u955c\u6280\u672f\u53ef\u7528\u4e8e\u786e\u5b9a\u5355\u4e2a\u91d1\u5c5e\u539f\u5b50\u7684\u5b58\u5728\u53ca\u5176\u5728\u8f7d\u4f53\u8868\u9762\u7ed3\u6784\u4e2d\u7684\u4f4d\u7f6e\u4ee5\u53ca\u7a7a\u95f4\u5206\u5e03\u5c24\u5176\u9002\u7528\uff0c\u5bf9\u4e8e\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u5408\u6210\u65b9\u6cd5\u7684\u53d1\u5c55\u548c\u4f18\u5316\u662f\u5fc5\u4e0d\u53ef\u5c11\u7684\u3002\u56fe8\u5217\u4e3e\u4e86\u51e0\u79cd\u4ee5\u7403\u5dee\u7535\u955c\u786e\u5b9a\u7684\u5355\u539f\u5b50\u50ac\u5316\u5242\u7684\u7403\u5dee\u7535\u955c\u7167\u7247\uff0c\u5176\u767d\u8272\u9ad8\u4eae\u7684\u539f\u5b50\u7ea7\u4eae\u70b9\u5373\u4e3a\u9644\u7740\u4e8e\u78b3\u57fa\u5e95\u7684\u5355\u539f\u5b50\u50ac\u5316\u5242 [5]<\/sup>\u3002<\/p>\n

\u56fe8 \u4e0d\u540c\u5355\u539f\u5b50\u9644\u7740\u4e8eC\u57fa\u5e95\u7684\u7403\u5dee\u7535\u955c\u7167\u7247\u3002<\/p>\n

\"\"<\/p>\n

2. \u8c31\u5b66\u6280\u672f<\/strong><\/p>\n

EXAFS\u548cXANES\u6280\u672f\u88ab\u5e7f\u6cdb\u5e94\u7528\u4e8e\u8d1f\u8f7d\u578b\u91d1\u5c5e\u7eb3\u7c73\u9897\u7c92\u6216\u8005\u56e2\u7c07\u7684\u8868\u5f81\u3002EXAFS\u5149\u8c31\u8868\u5f81\u91d1\u5c5e-\u91d1\u5c5e\u914d\u4f4d\u6570\u53ef\u7528\u4e8e\u6709\u6548\u786e\u5b9a\u5355\u539f\u5b50\u50ac\u5316\u5242\u662f\u5426\u5408\u6210\u6210\u529f\u3002\u6839\u636e\u5355\u539f\u5b50\u50ac\u5316\u5242\u5b9a\u4e49\uff0c\u5728EXAFS\u4e2d\uff0c\u6d3b\u6027\u4f4d\u70b9\u4e2d\u7684\u91d1\u5c5e-\u91d1\u5c5e\u952e\u662f\u4e0d\u5b58\u5728\u7684\u3002\u56e0\u6b64\uff0c\u5982\u679cEXAFS\u6570\u636e\u4e0d\u5305\u62ec\u4efb\u4f55\u5173\u4e8e\u91d1\u5c5e-\u91d1\u5c5e\u952e\u7684\u4fe1\u606f\uff0c\u4fbf\u53ef\u57fa\u672c\u63a8\u65ad\u53ea\u6709\u5355\u4e2a\u91d1\u5c5e\u539f\u5b50\u5b58\u5728\u4e8e\u50ac\u5316\u5242\u3002<\/p>\n

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\u56fe9 \u5355\u539f\u5b50Pt\u50ac\u5316\u5242EXAFS\u548cXANES\u5206\u6790\u3002<\/p>\n

\"\"<\/p>\n

\u4e94\u3001\u5c0f\u7ed3<\/strong><\/p>\n

\u5f00\u53d1\u9ad8\u6548\u3001\u8010\u7528\u3001\u7ecf\u6d4e\u7684\u7535\u50ac\u5316\u5242\u5bf9\u7535\u5316\u5b66\u80fd\u91cf\u8f6c\u6362\u6280\u672f\u7684\u53d1\u5c55\u548c\u5546\u4e1a\u5e94\u7528\u5177\u6709\u91cd\u8981\u610f\u4e49\u3002\u7136\u800c\uff0c\u8fd9\u4ecd\u7136\u662f\u4e00\u4e2a\u5de8\u5927\u7684\u6311\u6218\u3002\u8fd1\u5e74\u6765\uff0c\u901a\u8fc7\u7a7a\u4f4d\u7f3a\u9677\u951a\u5b9a\u7b56\u7565\u3001\u7a7a\u95f4\u9650\u57df\u7b56\u7565\u3001\u914d\u4f4d\u7b56\u7565\u7b49\u624b\u6bb5\uff0c\u7814\u7a76\u8005\u5236\u5907\u5e76\u62a5\u9053\u4e86\u8bb8\u591a\u5148\u8fdb\u7684\u5355\u539f\u5b50\u7535\u50ac\u5316\u5242\uff0c\u5e76\u5177\u6709\u826f\u597d\u7684\u6d3b\u6027\u3001\u9009\u62e9\u6027\u548c\u7a33\u5b9a\u6027\u3002\u8fd9\u4e9b\u5355\u539f\u5b50\u50ac\u5316\u5242\u5728CO2<\/sub>RR\u3001ORR\u3001HER\u7b49\u5173\u952e\u80fd\u91cf\u8f6c\u6362\u53cd\u5e94\u53d1\u6325\u4e86\u4f18\u5f02\u7684\u6027\u80fd\u3002\u6b64\u5916\uff0c\u7814\u7a76\u8005\u901a\u8fc7\u7403\u5dee\u7535\u955c\u53caEXAFS\u3001XANES\u6280\u672f\u7b49\u8868\u5f81\u4e86\u5355\u539f\u5b50\u50ac\u5316\u5242\u5728\u50ac\u5316\u9886\u57df\u7684\u673a\u7406\uff0c\u6709\u6548\u5730\u8bc1\u660e\u4e86\u5355\u539f\u5b50\u50ac\u5316\u5242\u6240\u5177\u6709\u7684\u5de8\u5927\u7684\u6f5c\u529b\u3002<\/p>\n

\u53c2\u8003\u6587\u732e<\/strong><\/p>\n

[1] J. Gu, C.-S. Hsu, L. Bai, H.M. Chen, X. Hu, Atomically dispersed Fe3+ sites catalyze efficient CO2 electroreduction to CO, Science, 364 (2019) 1091-1094.<\/p>\n

[2] C. Zhao, Y. Wang, Z. Li, W. Chen, Q. Xu, D. He, D. Xi, Q. Zhang, T. Yuan, Y. Qu, Solid-diffusion synthesis of single-atom catalysts directly from bulk metal for efficient CO2 reduction, Joule, 3 (2019) 584-594.<\/p>\n

[3] Y. Pan, R. Lin, Y. Chen, S. Liu, W. Zhu, X. Cao, W. Chen, K. Wu, W.-C. Cheong, Y. Wang, Design of single-atom Co\u2013N5 catalytic site: a robust electrocatalyst for CO2 reduction with nearly 100% CO selectivity and remarkable stability, J Am Chem Soc, 140 (2018) 4218-4221.<\/p>\n

[4] Z. Lu, B. Wang, Y. Hu, W. Liu, Y. Zhao, R. Yang, Z. Li, J. Luo, B. Chi, Z. Jiang, An Isolated Zinc\u2013Cobalt Atomic Pair for Highly Active and Durable Oxygen Reduction, Angewandte Chemie, 131 (2019) 2648-2652.<\/p>\n

[5] L. Zhao, Y. Zhang, L.-B. Huang, X.-Z. Liu, Q.-H. Zhang, C. He, Z.-Y. Wu, L.-J. Zhang, J. Wu, W. Yang, Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts, Nat Commun, 10 (2019) 1278.<\/p>\n

[6] L. Zhang, L. Han, H. Liu, X. Liu, J. Luo, Potential\u2010cycling synthesis of single platinum atoms for efficient hydrogen evolution in neutral media, Angewandte Chemie International Edition, 56 (2017) 13694-13698.<\/p>\n

[7] H. Fei, J. Dong, M.J. Arellano-Jim\u00e9nez, G. Ye, N.D. Kim, E.L. Samuel, Z. Peng, Z. Zhu, F. Qin, J. Bao, Atomic cobalt on nitrogen-doped graphene for hydrogen generation, Nat Commun, 6 (2015) 8668.<\/p>\n

[8] Z. Du, X. Chen, W. Hu, C. Chuang, S. Xie, A. Hu, W. Yan, X. Kong, X. Wu, H. Ji, Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium\u2013Sulfur Batteries, J Am Chem Soc, 141 (2019) 3977-3985.<\/p>\n

[9] Y. Chen, S. Ji, C. Chen, Q. Peng, D. Wang, Y. Li, Single-atom catalysts: synthetic strategies and electrochemical applications, Joule, 2 (2018) 1242-1264.<\/p>\n

[10] G. Liu, A.W. Robertson, M.M.-J. Li, W.C. Kuo, M.T. Darby, M.H. Muhieddine, Y.-C. Lin, K. Suenaga, M. Stamatakis, J.H. Warner, MoS 2 monolayer catalyst doped with isolated Co atoms for the hydrodeoxygenation reaction, Nature chemistry, 9 (2017) 810.<\/p>\n

[11] H.J. Qiu, Y. Ito, W. Cong, Y. Tan, P. Liu, A. Hirata, T. Fujita, Z. Tang, M. Chen, Nanoporous Graphene with Single\u2010Atom Nickel Dopants: An Efficient and Stable Catalyst for Electrochemical Hydrogen Production, Angewandte Chemie International Edition, 54 (2015) 14031-14035.<\/p>\n

[12] Y. Chen, S. Ji, Y. Wang, J. Dong, W. Chen, Z. Li, R. Shen, L. Zheng, Z. Zhuang, D. Wang, Isolated single iron atoms anchored on N\u2010doped porous carbon as an efficient electrocatalyst for the oxygen reduction reaction, Angewandte Chemie International Edition, 56 (2017) 6937-6941.<\/p>\n

[13] Y. Hou, M. Qiu, M.G. Kim, P. Liu, G. Nam, T. Zhang, X. Zhuang, B. Yang, J. Cho, M. Chen, Atomically dispersed nickel\u2013nitrogen\u2013sulfur species anchored on porous carbon nanosheets for efficient water oxidation, Nat Commun, 10 (2019) 1392.<\/p>\n

[14] B. Qiao, A. Wang, X. Yang, L.F. Allard, Z. Jiang, Y. Cui, J. Liu, J. Li, T. Zhang, Single-atom catalysis of CO oxidation using Pt 1\/FeO x, Nature chemistry, 3 (2011) 634.<\/p>\n

\u5f80\u671f\u56de\u987e\uff1a<\/strong><\/p>\n

\u8bfb\u4e66\u7b14\u8bb0\uff08Nature Communications\uff09 \uff1aDNA\u7535\u50ac\u5316\u5242\u4f60\u53ef\u66fe\u542c\u8fc7\uff1f<\/a><\/p>\n

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\u90a3\u4e9b\u5e74\uff0c\u9876\u520aScience\u4e0a\u7535\u50ac\u5316\u9886\u57df\u7684\u7cbe\u534e\uff0c\u4f60\u6709\u6ca1\u6709\u9519\u8fc7\uff1f<\/a><\/p>\n

\u7535\u50ac\u5316\u65b0\u5ba0\u4e4b\u5e38\u6e29\u5e38\u538b\u6c2e\u8fd8\u539f\uff08NRR\uff09\uff0c\u6700\u5168NRR\u4ecb\u7ecd\uff0c\u4f60\u60f3\u8981\u7684\u90fd\u5728\u8fd9\uff01<\/a><\/p>\n

\u672c\u6587\u7cfbaishou\u4f9b\u7a3f\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: tougao@cailiaoren.com.<\/p>\n

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