{"id":227659,"date":"2021-09-24T06:30:39","date_gmt":"2021-09-23T22:30:39","guid":{"rendered":"\/\/m.iemloyee.com\/?p=227659"},"modified":"2021-09-23T18:38:55","modified_gmt":"2021-09-23T10:38:55","slug":"%e4%b9%94%e4%b8%96%e7%92%8b%e5%9b%a2%e9%98%9fnature-energy%ef%bc%9a%e4%ba%9a%e9%93%81%e6%b0%b0%e5%8c%96%e9%95%8d%e4%bd%9c%e4%b8%ba%e9%ab%98%e6%80%a7%e8%83%bd%e5%b0%bf%e7%b4%a0%e6%b0%a7%e5%8c%96","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=227659","title":{"rendered":"\u4e54\u4e16\u748b\u56e2\u961fNature Energy\uff1a\u4e9a\u94c1\u6c30\u5316\u954d\u4f5c\u4e3a\u9ad8\u6027\u80fd\u5c3f\u7d20\u6c27\u5316\u7535\u50ac\u5316\u5242"},"content":{"rendered":"

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

\u7535\u50ac\u5316\u5c3f\u7d20\u6c27\u5316\u53cd\u5e94(UOR)\u5728\u4e00\u7cfb\u5217\u4e0e\u80fd\u6e90\u76f8\u5173\u7684\u5e94\u7528\u548c\u88c5\u7f6e\u4e2d\u5177\u6709\u91cd\u8981\u610f\u4e49\u3002\u5728\u5927\u591a\u6570\u60c5\u51b5\u4e0b\uff0c\u78b1\u6027\u4ecb\u8d28\u4e2d\u7684UOR\u662f\u4e00\u4e2a\u516d\u7535\u5b50-\u8d28\u5b50(\u6216\u7f9f\u57fa)\u8026\u5408\u8f6c\u79fb\u6b65\u9aa4\uff0cCO(NH2<\/sub>)2<\/sub>+6OH–<\/sup>\u2192N2<\/sub>+CO2<\/sub>+5H2<\/sub>O+6e–<\/sup>\uff0c\u5e73\u8861\u7535\u4f4d(E\u00b0)\u4e3a0.37V (\u76f8\u5bf9\u4e8e\u53ef\u9006\u6c22\u7535\u6781(RHE))\u3002\u76ee\u524d\uff0c\u7531\u4e8e6e–<\/sup>\u8f6c\u79fb\u8fc7\u7a0b\u590d\u6742\uff0cUOR\u7684\u8fc7\u7535\u4f4d\u4ecd\u7136\u5f88\u9ad8\u3002\u7136\u800c\uff0cUOR\u4f5c\u4e3a\u53d6\u4ee3\u4f20\u7edf\u6790\u6c27\u53cd\u5e94(OER)\u7684\u7406\u60f3\u534a\u9633\u6781\u53cd\u5e94\uff0c\u5728\u8282\u80fd\u578b\u6c34\u7535\u89e3\u5236\u6c22\u4e2d\u4ecd\u5177\u6709\u5de8\u5927\u7684\u6f5c\u529b\u3002\u4e0eOER\u76f8\u6bd4\uff0cUOR\u7684\u52a8\u529b\u5b66\u66f4\u52a0\u7f13\u6162\uff0c\u56e0\u4e3a\u8fc7\u7a0b\u4e2d\u9700\u8981\u4f20\u9012\u66f4\u591a\u7684\u7535\u5b50\uff0c\u56e0\u6b64\u9700\u8981\u9ad8\u6027\u80fd\u7684\u50ac\u5316\u5242\u6765\u964d\u4f4e\u8fc7\u7535\u4f4d\uff0c\u4ece\u800c\u5b9e\u73b0\u9ad8\u6548\u7684\u5668\u4ef6\u3002\u7136\u800c\uff0c\u6700\u8fd1\u5f00\u53d1\u7684\u57fa\u4e8eNi\u6c22\u6c27\u5316\u7269\u3001\u6c27\u5316\u7269\u3001\u786b\u5316\u7269\u3001\u81a6\u5316\u7269\u7b49\u7684\u975e\u8d35\u91d1\u5c5eUOR\u50ac\u5316\u5242\uff0c\u7531\u4e8e\u8fc7\u7535\u4f4d\u9ad8\u3001\u7535\u6d41\u5bc6\u5ea6\u4f4e\u3001\u7a33\u5b9a\u6027\u4e0d\u591f\u597d\u7b49\u539f\u56e0\uff0c\u5176\u50ac\u5316\u6027\u80fd\u5e76\u4e0d\u80fd\u6ee1\u8db3\u5b9e\u9645\u5e94\u7528\u7684\u8981\u6c42\u3002\u8fd9\u79cd\u8f83\u5dee\u7684\u6027\u80fd\u53ef\u80fd\u662f\u7531\u4e8e\u56fa\u6709\u7684\u53cd\u5e94\u673a\u7406\u6240\u81f4\u3002\u7279\u522b\u5730\uff0c\u5bf9\u4e8e\u7814\u7a76\u6700\u591a\u7684\u954d\u57fa\u6750\u6599\uff0c\u5728UOR\u5f00\u59cb\u524d(\u4f8b\u59821.40 V )\uff0c\u50ac\u5316\u5242\u4e0d\u53ef\u907f\u514d\u5730\u8981\u7ecf\u5386\u4e00\u4e2a\u81ea\u6c27\u5316\u8fc7\u7a0b\uff0c\u5728\u8868\u9762\u5f62\u6210Ni<\/b><\/strong>3+<\/b><\/sup><\/strong>\u6001NiOOH\u884d\u751f\u7269(\u901a\u5e38\u53d1\u751f\u57281.36 V\u9644\u8fd1)\uff0c\u7136\u540e\u4f5c\u4e3aUOR\u7684\u76f4\u63a5\u6d3b\u6027\u4f4d\u70b9\u3002\u56e0\u6b64\uff0c\u5c3d\u7ba1\u7814\u7a76\u4eba\u5458\u5df2\u7ecf\u5f00\u53d1\u4e86\u591a\u79cd\u5177\u6709\u4e0d\u540c\u7ec4\u6210\u548c\u7ed3\u6784\u7684\u50ac\u5316\u5242\uff0c\u4f46\u5927\u591a\u6570\u50ac\u5316\u5242\u90fd\u6d89\u53caNiOOH\uff0c\u9650\u5236\u4e86\u6d3b\u6027\u3002<\/b><\/strong><\/p>\n

\"\"<\/p>\n

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

\u8fd1<\/b><\/strong>\u65e5\uff0c\u5b89\u5fbd\u5927\u5b66\u3001\u4e2d\u56fd\u79d1\u6280\u5927\u5b66\u3001\u6fb3\u5927\u5229\u4e9a<\/b><\/strong>\u963f\u5fb7\u83b1\u5fb7<\/b><\/strong>\u5927\u5b66<\/b><\/strong>\u9648\u5e73\/\u5218\u5e86\u534e\/\u4e54\u4e16\u748b\u4f5c\u4e3a\u5171\u540c\u901a\u8baf\u4f5c\u8005<\/b><\/strong>\u5408\u6210\u4e86\u4e00\u79cd\u8d1f\u8f7d\u5728\u6ce1\u6cab\u954d\u4e0a\u7684\u4e00\u79cd\u7531\u666e\u9c81\u58eb\u84dd\u7c7b\u4f3c\u7269\u4e4b\u4e00\u7684\u4e9a\u94c1\u6c30\u5316\u954d(Ni<\/b><\/strong>2<\/b><\/sub><\/strong>Fe(CN)<\/b><\/strong>6<\/b><\/sub><\/strong>)\u50ac\u5316\u5242<\/b><\/strong>\uff0c\u8be5\u50ac\u5316\u5242\u6bd4\u5e38\u89c4\u954d\u57fa\u50ac\u5316\u5242\u5177\u6709\u66f4\u9ad8\u7684\u6d3b\u6027\u548c\u66f4\u597d\u7684\u7a33\u5b9a\u6027\u9a71\u52a8UOR\u3002\u4e0e\u73b0\u6709\u50ac\u5316\u5242\u76f8\u6bd4\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u4e0a\u7684\u5c3f\u7d20\u6c27\u5316\u5728\u6750\u6599\u81ea\u6c27\u5316\u4e4b\u524d\u8fdb\u884c\uff0c\u4ece\u800c\u907f\u514d\u4e86\u9ad8\u4ef7\u6001\u7684Ni3+<\/sup>(\u4f8b\u5982NiOOH)\u7684\u751f\u6210\uff0c\u63d0\u9ad8\u4e86\u50ac\u5316\u6d3b\u6027\u548c\u7a33\u5b9a\u6027\u3002\u7ed3\u679c\u8868\u660e\uff0cUOR\u673a\u7406\u5305\u62ec\u5c3f\u7d20\u5230NH3<\/sub>\u7684\u5316\u5b66\u8fc7\u7a0b\u548cNH3<\/sub>\u5230N2<\/sub>\u5728\u50ac\u5316\u5242\u8868\u9762\u4e0d\u540c\u4f4d\u7f6e\u7684\u7535\u5316\u5b66\u8fc7\u7a0b\uff0c\u8fd9\u4e0e\u76ee\u524d\u6240\u7406\u89e3\u7684\u673a\u7406\u622a\u7136\u4e0d\u540c\u3002\u6b64\u5916\uff0c\u672c\u5de5\u4f5c\u7684\u53cc\u7535\u6781\u5b9e\u9a8c\u8868\u660e\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u9a71\u52a8\u7684UOR\u8fc7\u7a0b\u53ef\u4ee5\u5728\u9ad8\u7535\u6d41\u5bc6\u5ea6\u4e0b\u66ff\u4ee3\u5e38\u89c4\u6c34\u7535\u89e3\u3002\u76f8\u5173\u6210\u679c\u4ee5\u9898\u4e3a\u201cNickel ferrocyanide as a high-performance urea oxidation electrocatalyst\u201d\u53d1\u8868\u5728\u4e86Nature Energy\u4e0a\u3002<\/p>\n

\u56fe\u6587\u89e3\u6790<\/b><\/strong><\/p>\n

\u4e00\u3001\u7406\u5316\u6027\u80fd\u53caUOR\u6027\u80fd\u8bc4\u4f30<\/b><\/strong>\u3002<\/b><\/strong><\/p>\n

\u672c\u5de5\u4f5c\u91c7\u7528\u81ea\u7ec4\u88c5\u6cd5\u5728\u6ce1\u6cab\u954d\u4e0a\u5236\u5907\u4e86\u5178\u578b\u7684Ni2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u3002\u626b\u63cf\u7535\u5b50\u663e\u5fae\u955c(SEM)\u56fe\u50cf\u663e\u793a\uff0c\u6240\u5408\u6210\u7684\u4ea7\u7269\u662f\u7531\u7ec4\u88c5\u5728\u6ce1\u6cab\u954d\u8868\u9762\u7684\u7eb3\u7c73\u7acb\u65b9\u4f53\u4e0e\u5355\u5c42\u6d82\u5c42\u7ec4\u6210\u3002\u900f\u5c04\u7535\u5b50\u663e\u5fae\u955c(TEM)\u56fe\u50cf\u663e\u793a\u4ea7\u7269\u4e3a\u9ad8\u5ea6\u7ed3\u6676\u7684\u7acb\u65b9\u7eb3\u7c73\u9897\u7c92\u3002\u672c\u5de5\u4f5c\u5bf9Ni2<\/sub>Fe(CN)6<\/sub>\u7c89\u672b\u7684X\u5c04\u7ebf\u7c89\u672b\u884d\u5c04(XRD)\u56fe\u8c31\u7684\u8fdb\u884c\u4e86\u5206\u6790\uff0c\u53d1\u73b0Fe\u539f\u5b50\u4e0eCN-\u4e2d\u7684\u78b3\u539f\u5b50\u914d\u4f4d\uff0cNi\u539f\u5b50\u6709\u4e24\u79cd\u914d\u4f4d\u5f62\u5f0f\uff1a\u4e00\u79cd\u4e0eCN-\u4e2d\u7684N\u539f\u5b50\u914d\u4f4d\uff0c\u53e6\u4e00\u79cd\u5355\u72ec\u4f4d\u4e8e\u4e2d\u5fc3\u3002\u6709\u8da3\u7684\u662f\uff0c\u57281\u5c0f\u65f6\u7684UOR\u8fc7\u7a0b\u4e2d\uff0cFe2+<\/sup>\u548cNi2+<\/sup>\u90fd\u6ca1\u6709\u88ab\u6c27\u5316\u6210FeOOH\u548cNiOOH\uff0c\u8fd9\u4e0e\u5176\u4ed6\u954d\u57fa\u50ac\u5316\u5242\u62a5\u9053\u7684\u4e0d\u540c\u3002\u7531\u4e8e\u4eba\u4f53\u5c3f\u6db2\u4e2d\u542b\u67092~2.5wt %\u7684\u5c3f\u7d20(\u6469\u5c14\u6d53\u5ea6\u4e3a~0.33M)\uff0c\u6545\u672c\u5de5\u4f5c\u7535\u89e3\u65f6\u9009\u75280.33M\u5c3f\u7d20\u3002\u901a\u8fc7\u7ebf\u6027\u626b\u63cf\u4f0f\u5b89(LSV)\u53ef\u77e5\uff0c\u4f18\u5316\u540e\u7684Ni2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u4e0a\u7684UOR\u6bd4OER\u8868\u73b0\u51fa\u66f4\u8d1f\u7684\u8d77\u59cb\u7535\u4f4d\u3002Ni<\/b><\/strong>2<\/b><\/sub><\/strong>Fe(CN)<\/b><\/strong>6<\/b><\/sub><\/strong>\u7535\u50ac\u5316\u5242\u7684\u9ad8\u6027\u80fd\u53ef\u5f52\u56e0\u4e8e\u5176Ni<\/b><\/strong>2+<\/b><\/sup><\/strong>\u7684\u7a33\u5b9a\u6027\u3002<\/b><\/strong>\u4e0e\u5927\u591a\u6570\u62a5\u9053\u7684\u954d\u57fa\u50ac\u5316\u5242\u4e0d\u540c\u7684\u662f\uff0c\u4f5c\u8005\u53d1\u73b0\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u4e0a\u7684\u5c3f\u7d20\u6c27\u5316\u7684\u7535\u4f4d\u6bd4\u50ac\u5316\u5242\u81ea\u6c27\u5316\u7535\u4f4d\u4f4e\uff0c\u4ece\u800c\u907f\u514d\u751f\u6210\u9ad8\u4ef7\u6001\u7684Ni3+<\/sup>(\u4f8b\u5982NiOOH)\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\u4e0eNi2<\/sub>Fe(CN)6<\/sub>\u76f8\u6bd4\uff0c\u53e6\u4e24\u79cd\u7c7b\u4f3c\u6c30\u5316\u7269Fe4<\/sub>[Fe(CN)6<\/sub>]3<\/sub>\u548cNi3<\/sub>[Co(CN)6<\/sub>]2<\/sub>\uff0c\u4ee5\u53ca\u53e6\u5916\u542bNi\u548cFe\u7684\u954d\u94c1\u5c42\u72b6\u53cc\u6c22\u6c27\u5316\u7269\u5747\u8868\u73b0\u51fa\u66f4\u5dee\u7684\u6d3b\u6027\u3002\u56e0\u6b64\uff0c\u4f5c\u8005\u63a8\u65ad\u89c2\u5bdf\u5230\u7684Ni2<\/sub>Fe(CN)6<\/sub>\u7684\u9ad8\u6027\u80fd\u662f\u7531\u4e8eNi2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u4e2dNi\u548cFe\u4e24\u4e2a\u6d3b\u6027\u4f4d\u70b9\u7684\u534f\u540c\u4f5c\u7528<\/b><\/strong>\u6240\u81f4\u3002\u52a8\u529b\u5b66\u7814\u7a76\u8868\u660e\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u4e0a\u7684UOR\u8fc7\u7a0b\u4e0e\u5c3f\u7d20\u6d53\u5ea6\u65e0\u5173(\u56fe1f )\uff0c\u8fd9\u4e0e\u62a5\u9053\u7684Ni\u57fa\u7535\u50ac\u5316\u5242\u4e00\u81f4\u3002\u76f8\u53cd\uff0cUOR\u5bf9KOH\u7684\u7528\u91cf\u6709\u5f88\u5f3a\u7684\u4f9d\u8d56\u6027\u3002<\/p>\n

\"\"<\/p>\n

\u56fe1. Ni2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u5728\u4e09\u7535\u6781\u7535\u6c60\u4e0a\u7684UOR\u6027\u80fd\u8bc4\u4ef7<\/p>\n

\u4e8c\u3001Ni<\/b><\/strong>2<\/b><\/sub><\/strong>Fe(CN)<\/b><\/strong>6<\/b><\/sub><\/strong>\u4e0e\u5e38\u89c4NiC<\/b><\/strong>2<\/b><\/sub><\/strong>O<\/b><\/strong>4<\/b><\/sub><\/strong>\u50ac\u5316\u5242\u7684\u6bd4\u8f83\u3002<\/b><\/strong><\/p>\n

\u4f5c\u4e3a\u5bf9\u7167\uff0c\u672c\u5de5\u4f5c\u5236\u5907\u4e86\u4e00\u79cd\u4f20\u7edf\u7684\u8349\u9178\u954d(NiC2O4)\u50ac\u5316\u5242\uff0c\u5e76\u6839\u636e\u4e00\u7cfb\u5217\u539f\u4f4d\u5149\u8c31\u6d4b\u91cf\u7ed3\u679c\u5c06\u5176\u4e0eNi2Fe(CN)6\u8fdb\u884c\u4e86\u6bd4\u8f83\uff0c\u4ee5\u9610\u660eUOR\u7684\u673a\u7406\u3002SEM\u548cXRD\u663e\u793a\uff0cNiC2O4\u4ee5\u5fae\u7c73\u5927\u5c0f\u7684\u5355\u659c\u7c92\u5b50\u7684\u5f62\u5f0f\u5b58\u5728\u3002\u5728Ni2<\/sub>Fe(CN)6<\/sub>\u7684\u62c9\u66fc\u5149\u8c31\u4e2d\uff0c2100\u548c2140 cm-1<\/sup>\u5904\u7684\u4e24\u4e2a\u5f3a\u5cf0\u662f\u6c30\u5316\u4f38\u7f29\u632f\u52a8\uff0c\u800c250\u548c348 cm-1<\/sup>\u5904\u7684\u5cf0\u5c5e\u4e8eNi-N\u4f38\u7f29\u632f\u52a8\uff0c510 cm-1<\/sup>\u5904\u7684\u5cf0\u5c5e\u4e8eFe-C\u4f38\u7f29\u632f\u52a8\u3002\u91cd\u8981\u7684\u662f\uff0c\u4e0d\u540c\u7535\u52bf\u4e0b\u7684\u62c9\u66fc\u5149\u8c31\u4e0e\u5f00\u8def\u7535\u52bf(OCP)\u4e0b\u7684\u76f8\u4f3c\u3002\u4e0e\u4e4b\u5bf9\u5e94\uff0c\u5728NiC2O4 UOR\u8fc7\u7a0b\u4e2d\uff0c\u5728\u9ad8\u7535\u4f4d\u4e0b\uff0c\u5728\u5f88\u77ed\u7684\u65f6\u95f4\u5185\u51fa\u73b0\u4e86473\u548c560cm–<\/sup>1<\/sup>\u7684NiOOH\u53cc\u5cf0\uff0c\u8868\u660e\u5176\u5bf9NiOOH\u7684\u90e8\u5206\u91cd\u6784\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\u5c3d\u7ba1Ni2<\/sub>Fe(CN)6<\/sub>\u6bd4NiC2<\/sub>O4<\/sub>\u8868\u73b0\u51fa\u4e86\u66f4\u9ad8\u7684\u7a33\u5b9a\u6027\uff0c\u4f46\u5b83\u57286\u5c0f\u65f6\u540e\u88ab\u8f6c\u5316\u4e3a\u6c22\u6c27\u5316\u954d\u884d\u751f\u7269\u3002\u4eceNi2Fe(CN)6\u50ac\u5316\u5242UOR\u6d4b\u8bd5\u524d\u540e\u7684TEM\u56fe\u50cf\u548c\u5143\u7d20\u6620\u5c04(Fe, Ni\u548cN)\u53ef\u4ee5\u770b\u51fa\uff0c\u5143\u7d20\u5728UOR\u524d\u540e\u57fa\u672c\u4e00\u81f4\uff0c\u56e0\u6b64\u6ca1\u6709\u8bc1\u636e\u8868\u660e\u5bccFe\/Ni\u6838\u58f3\u7ed3\u6784\u7684\u5f62\u6210\u3002\u4e0eNiC2<\/sub>O4<\/sub>\u50ac\u5316\u5242\u76f8\u6bd4\uff0c Ni2<\/sub>Fe (CN)6<\/sub>\u8868\u73b0\u51fa\u660e\u663e\u7684UOR\u6d3b\u6027\u589e\u5f3a\u3002Ni2<\/sub>Fe(CN)6<\/sub>\u00a0<\/sub>\u548cNiC2<\/sub>O4<\/sub>\u4e0e\u7535\u89e3\u8d28\u4e2dOH–<\/sup>\u6d53\u5ea6\u7684\u53cd\u5e94\u7ea7\u6570\u5206\u522b\u4e3a1.1\u548c1.75\u3002\u56e0\u6b64\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u7684\u8fd9\u79cd\u72ec\u7279\u7684\u52a8\u529b\u5b66\u5173\u7cfb\u9884\u793a\u7740\u53e6\u4e00\u79cd\u53cd\u5e94\u9014\u5f84\u3002\"\"<\/p>\n

\u56fe2. Ni2<\/sub>Fe(CN)6<\/sub>\u4e0e\u5e38\u89c4NiC2<\/sub>O4<\/sub>\u50ac\u5316\u5242\u7684\u6bd4\u8f83<\/p>\n

\u4e09\u3001\u57fa\u4e8e\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\u7684\u8ba1\u7b97\u3002<\/b><\/strong><\/p>\n

\u6839\u636e\u4e0a\u8ff0\u5206\u6790\uff0c\u672c\u5de5\u4f5c\u63d0\u51fa\u4e86UOR\u7684\u53cd\u5e94\u673a\u7406\uff0c\u5305\u62ec\u4e24\u4e2a\u9636\u6bb5\uff0c\u5373\u5c3f\u7d20\u2192NH3<\/sub>(CO(NH2<\/sub>)2<\/sub>+H2<\/sub>O\u2192CO2<\/sub>+2NH3<\/sub>)\u7684\u5316\u5b66\u8fc7\u7a0b\u548cNH3<\/sub>\u2192N2<\/sub>(2NH3<\/sub>+6OH–<\/sup>\u2192N2<\/sub>+6H2<\/sub>O+ 6e–<\/sup>)\u7684\u7535\u5316\u5b66\u8fc7\u7a0b\u3002\u7b2c\u4e00\u9636\u6bb5\u5305\u62ec\u5c3f\u7d20\u5438\u9644\u3001\u8131\u6c28\u3001\u8131\u78b3\u548cNH3<\/sub>\u8131\u9644\u56db\u4e2a\u6b65\u9aa4\u3002\u5728\u53cd\u5e94\u52a8\u529b\u5b66\u65b9\u9762\uff0cNi\u4f4d\u548cFe\u4f4d\u7684\u53cd\u5e94\u6d3b\u5316\u80fd\u0394G *\u53d8\u5316\u8d8b\u52bf\u76f8\u540c\u3002\u7b2c\u4e09\u4e2a\u57fa\u5143\u53cd\u5e94([M\u00b7OCONH2<\/sub>]ads<\/sub>\u2192[M\u00b7NH2<\/sub>]ads<\/sub>+CO2<\/sub>)\u4e3a\u70ed\u529b\u5b66\u9650\u5236\u6b65\u9aa4\u3002Ni\u4f4d\u88ab\u8ba4\u4e3a\u662f\u8be5\u6b65\u9aa4\u4e2d\u8f83\u4f18\u7684\u50ac\u5316\u4f4d\u3002\u5728\u53cd\u5e94\u52a8\u529b\u5b66\u65b9\u9762\uff0c\u5bf9\u4e8eNi\u4f4d\u548cFe\u4f4d\uff0c\u53cd\u5e94\u6d3b\u5316\u80fd\u0394G*\u5448\u73b0\u76f8\u540c\u7684\u53d8\u5316\u8d8b\u52bf\u3002\u5316\u5b66\u70ed\u529b\u5b66\u6570\u636e\u8868\u660e\uff0cFe\u4f4d\u4f18\u4e8eNi\u4f4d\uff0c\u6fc0\u6d3b\u80fd\u8868\u660eFe\u4f4d\u66f4\u5bb9\u6613\u514b\u670d\u80fd\u5792\u3002\u6839\u636e\u4e0a\u8ff0\u53cd\u5e94\u673a\u7406\uff0c\u672c\u5de5\u4f5c\u5047\u8bbeNi\u8d1f\u8d23\u5c06\u5c3f\u7d20\u8f6c\u5316\u4e3a\u6c28\u548c\u4e8c\u6c27\u5316\u78b3\uff0cFe\u8d1f\u8d23\u5c06\u6c28\u8f6c\u5316\u4e3a\u6c2e\u6c14\u3002DFT\u8ba1\u7b97\u63ed\u793a\u7684Ni\u548cFe\u4f4d\u4e4b\u95f4\u7684\u534f\u540c\u50ac\u5316\u4f5c\u7528\uff0c\u8bc1\u660e\u4e86Ni2<\/sub>Fe(CN)6<\/sub>\u4f18\u4e8e\u5176\u4ed6\u50ac\u5316\u5242\u7684\u673a\u7406\u3002DFT\u8ba1\u7b97\u9884\u6d4b\uff0cNH<\/b><\/strong>3<\/b><\/sub><\/strong>\u662fUOR\u8fc7\u7a0b\u4e2d\u7684\u5173\u952e\u53cd\u5e94\u4e2d\u95f4\u4f53\uff0c\u53ef\u5206\u4e3a\u5c3f\u7d20\u5230NH<\/b><\/strong>3<\/b><\/sub><\/strong>\u7684\u5316\u5b66\u53cd\u5e94\u548cNH<\/b><\/strong>3<\/b><\/sub><\/strong>\u5230N<\/b><\/strong>2<\/b><\/sub><\/strong>\u7684\u7535\u5316\u5b66\u53cd\u5e94\u4e24\u4e2a\u9636\u6bb5\u3002<\/b><\/strong><\/p>\n

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

\u56fe3. UOR\u5728Ni2<\/sub>Fe(CN)6<\/sub>\uff08011\uff09\u8868\u9762\u7684\u53cd\u5e94\u673a\u7406\u56fe<\/p>\n

<\/b>\u56db\u3001\u4e2d\u95f4\u4f53\u7684\u9274\u5b9a\u3002<\/b><\/strong><\/p>\n

\u4e3a\u4e86\u786e\u5b9aDFT\u8ba1\u7b97\u4e2d\u63d0\u51fa\u7684\u5173\u952e\u53cd\u5e94\u4e2d\u95f4\u4f53\uff0c\u672c\u5de5\u4f5c\u8fdb\u884c\u4e86\u539f\u4f4d\u540c\u6b65\u8f90\u5c04\u5085\u91cc\u53f6\u53d8\u6362\u7ea2\u5916(SR- FTIR)\u5206\u6790\u3002\u5bf9\u4e8eNi2<\/sub>Fe (CN)6<\/sub>\uff0c\u4e0eOCP\u5904\u7684\u8c31\u56fe\u76f8\u6bd4\uff0c\u5728UOR\u5de5\u4f5c\u7535\u4f4d\u4e0b\uff0c2925cm-1<\/sup>\u548c1203cm-1<\/sup>\u5904\u51fa\u73b0\u4e86\u4e24\u4e2a\u660e\u663e\u7684\u5438\u6536\u5e26\uff0c\u5206\u522b\u53ef\u5f52\u5c5e\u4e3a*N=NH2+<\/sup>\u7684N-H\u4f38\u7f29\u632f\u52a8\u548c*OCONH2<\/sub>\u7684C-O\u4f38\u7f29\u632f\u52a8\u3002\u968f\u7740\u7535\u4f4d\u7684\u589e\u52a0\uff0c\u8fd9\u4e24\u4e2a\u7279\u5f81\u5cf0\u53d8\u5f3a\uff0c\u8c10\u6ce2\u632f\u52a8\u9891\u7387\u7684\u6a21\u62df\u7ed3\u679c\u4e5f\u8868\u660e\uff0c\u8fd9\u4e24\u4e2a\u5cf0\u53ef\u4ee5\u5f52\u7ed3\u4e3a*N=NH2+<\/sup>\u548c*OCONH2<\/sub>\u3002\u56e0\u6b64\u53ef\u5f97\u51fa\u7ed3\u8bba\uff0c\u8fd9\u4e24\u4e2a\u4e2d\u95f4\u4ea7\u7269\u662f\u5728UOR\u8fc7\u7a0b\u4e2d\u4ea7\u751f\u7684\u3002\u4f5c\u4e3a\u5bf9\u7167\uff0c\u672c\u5de5\u4f5c\u8fd8\u5bf9NiC2<\/sub>O4<\/sub>\u7535\u50ac\u5316\u5242\u8fdb\u884c\u4e86\u5206\u6790\uff0c\u4ee5\u8bc6\u522b\u4e0d\u540c\u7684\u53cd\u5e94\u4e2d\u95f4\u4f53\u3002\u672c\u5de5\u4f5c\u53d1\u73b0\uff0c\u5728UOR\u5de5\u4f5c\u7535\u4f4d\u4e0b\uff0c\u57282136 cm-1<\/sup>\u5904\u51fa\u73b0\u4e86\u660e\u663e\u7684CNO–<\/sup>\u5438\u6536\u5e26\u3002\u5728<\/b><\/strong>NiC2<\/sub>O4<\/sub>\u7535\u50ac\u5316\u5242\u7684\u8c31\u56fe\u4e2d\u6ca1\u6709\u89c2\u5bdf\u5230*N=NH2<\/sub>+<\/sup>\u4e2d\u95f4\u4f53\u4e2d\u7684N-H\u4f38\u7f29\u632f\u52a8\u548c* OCONH2<\/sub>\u4e2d\u95f4\u4f53\u4e2d\u7684C-O\u4f38\u7f29\u632f\u52a8\u3002\u8fd9\u4e9b\u6bd4\u8f83\u6e05\u695a\u5730\u8868\u660e\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u4e0a\u7684UOR\u673a\u7406\u4e0e\u4f20\u7edf\u7684Ni\u57fa\u50ac\u5316\u5242\u4e0d\u540c\u3002\u5728\u8fd9\u4e00\u9636\u6bb5\uff0c\u52a8\u529b\u5b66\u5206\u6790\u3001DFT\u8ba1\u7b97\u548c\u539f\u4f4dSR-FTIR\u5149\u8c31\u6570\u636e\u7684\u7ed3\u5408\u8868\u660e\uff0cNi<\/b><\/strong>2<\/b><\/sub><\/strong>Fe(CN)<\/b><\/strong>6<\/b><\/sub><\/strong>\u5728\u6ca1\u6709NiOOH\u751f\u6210\u7684\u60c5\u51b5\u4e0b\u53d1\u751f\u4e86\u53e6\u4e00\u79cdUOR\u673a\u5236\uff0c\u5305\u62ec\u4ece\u5c3f\u7d20\u5230NH<\/b><\/strong>3<\/b><\/sub><\/strong>\u7684\u5316\u5b66\u8fc7\u7a0b\u548c\u5728\u4e24\u4e2a\u4e0d\u540c\u7684\u6d3b\u6027\u4f4d\u70b9\u4eceNH<\/b><\/strong>3<\/b><\/sub><\/strong>\u5230N<\/b><\/strong>2<\/b><\/sub><\/strong>\u7684\u7535\u5316\u5b66\u8fc7\u7a0b\u3002<\/b><\/strong><\/p>\n

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

\u56fe4. \u4e0d\u540c\u6761\u4ef6\u4e0b\u50ac\u5316\u5242\u7684\u539f\u4f4dSR-FTIR\u5149\u8c31<\/p>\n

\u4e94\u3001UOR\u9a71\u52a8\u7684\u8282\u80fd\u7cfb\u7edf\u3002<\/b><\/strong><\/p>\n

\u4e3a\u4e86\u901a\u8fc7Ni2<\/sub>Fe(CN)6<\/sub>\u50ac\u5316\u5242\u5efa\u7acbUOR\/\/HER\u8282\u80fd\u4f53\u7cfb\uff0c\u672c\u5de5\u4f5c\u4ee5Ni2<\/sub>Fe(CN)6<\/sub>\u4e3a\u9633\u6781\uff0c\u5728\u542b\u67091M KOH\u548c0.33 M\u5c3f\u7d20\u7684\u7535\u89e3\u6db2\u4e2d\u7ec4\u88c5\u4e86UOR\/\/HER\u7535\u89e3\u69fd\u3002\u4e3a\u83b7\u5f9710\u548c100 mAcm-2<\/sup>\u7684\u7535\u6d41\u5bc6\u5ea6\uff0c\u5c3f\u7d20\u7535\u89e3\u9700\u8981\u7684\u69fd\u7535\u538b\u5206\u522b\u4e3a1.38\u548c1.50V\uff0c\u6c34\u7535\u89e3\u9700\u8981\u7684\u69fd\u7535\u538b\u5206\u522b\u4e3a1.56\u548c1.85V\u3002\u53ef\u4ee5\u53d1\u73b0UOR\u5de5\u827a\u5728Ni<\/b><\/strong>2<\/b><\/sub><\/strong>Fe(CN)<\/b><\/strong>6<\/b><\/sub><\/strong>\u7535\u50ac\u5316\u5242\u4e0a\u66f4\u4e3a\u8282\u80fd\u3002<\/b><\/strong>\u6b64\u5916\uff0c\u8be5UOR\/\/HER\u7684H2<\/sub>\u4ea7\u91cf\u7a33\u5b9a\uff0c\u6cd5\u62c9\u7b2c\u6548\u7387\u8d85\u8fc790%\u3002\u9664\u751f\u4ea7H2<\/sub>\u5916\uff0c\u8be5\u8282\u80fd\u7cfb\u7edf\u8fd8\u53ef\u5e94\u7528\u4e8e\u7531Ni2<\/sub>Fe(CN)6<\/sub>\u9633\u6781\u548c\u4e2d\u5b54\u70ad(CMK-3<\/sup>)\u9634\u6781\u7ec4\u6210\u7684UOR\/\/2e–<\/sup>ORR\u6d41\u52a8\u76f8\u7535\u89e3\u6c60\u3002\u76ee\u524d\uff0c\u901a\u8fc72e<\/b><\/strong>–<\/b><\/sup><\/strong>\u00a0ORR\u539f\u4f4d\u7535\u5316\u5b66\u751f\u4ea7H<\/b><\/strong>2<\/b><\/sub><\/strong>O<\/b><\/strong>2<\/b><\/sub><\/strong>\u5df2\u6210\u4e3a\u4e00\u79cd\u5f88\u6709\u524d\u666f\u7684\u65b9\u6cd5\uff0c\u56e0\u4e3a\u5b83\u53ef\u4ee5\u964d\u4f4eH<\/b><\/strong>2<\/b><\/sub><\/strong>O<\/b><\/strong>2<\/b><\/sub><\/strong>\u8fd0\u8f93\u7684\u5371\u9669\u6027\u548c\u6210\u672c<\/b><\/strong>\u3002\u4f5c\u8005\u53d1\u73b0\uff0c\u4e0e\u6c34\u7535\u89e3\u76f8\u6bd4\uff0c<\/b><\/strong>\u5c3f\u7d20\u7535\u89e3\u9700\u8981\u66f4\u5c0f\u7684\u80fd\u91cf\u8f93\u5165\u6765\u6d88\u9664\u5c3f\u7d20\u548c\u8fc7\u6c27\u5316\u6c22\u7684\u751f\u6210\u3002<\/b><\/strong><\/p>\n

\"\"<\/p>\n

\u56fe5. \u5728H2<\/sub>\u548cH2<\/sub>O2<\/sub>\u7684\u8282\u80fd\u7cfb\u7edf\u4e2d\uff0cOER\u88abUOR\u53d6\u4ee3<\/p>\n

\u7ed3\u8bba\u4e0e\u5c55\u671b<\/b><\/strong><\/p>\n

\u603b\u7684\u6765\u8bf4\uff0c\u672c\u5de5\u4f5c\u91c7\u7528\u7b80\u5355\u6613\u6269\u5c55\u7684\u65b9\u6cd5\u5236\u5907\u4e86\u5177\u6709\u9ad8\u6d3b\u6027\u7684Ni2<\/sub>Fe(CN)6<\/sub>\u7535\u50ac\u5316\u5242\u7528\u4e8eUOR\u3002\u5b83\u663e\u793a\u51fa\u6bd4\u5176\u4ed6\u954d\u57faUOR\u7535\u50ac\u5316\u5242\u66f4\u597d\u7684\u7a33\u5b9a\u6027\u3002\u4f5c\u8005\u5bf9\u5176\u673a\u7406\u8fdb\u884c\u7814\u7a76\u53d1\u73b0\uff0c\u4e0e\u5927\u591a\u6570\u62a5\u9053\u7684\u7535\u50ac\u5316\u5242\u76f8\u6bd4\uff0cNi2<\/sub>Fe(CN)6<\/sub>\u4e0a\u7684UOR\u9014\u5f84\u66f4\u4e3a\u6709\u5229\u3002DFT\u7ed3\u679c\u8868\u660e\uff0c\u9ad8\u589e\u5f3a\u7684\u7535\u5316\u5b66\u6027\u80fd\u6e90\u4e8eNi2<\/sub>Fe(CN)6<\/sub>\u4e2dNi\u548cFe\u53cc\u6d3b\u6027\u4f4d\u7684\u534f\u540c\u4f5c\u7528\u3002Ni2<\/sub>Fe(CN)6<\/sub>\u4e0a\u7684\u9ad8\u6548UOR\u4e0e\u5e38\u89c4OER\u76f8\u6bd4\uff0c\u5176\u4f18\u70b9\u5728\u4e8e\u6240\u9700\u80fd\u91cf\u8f83\u5c11\uff0c\u540c\u65f6\u8fd8\u80fd\u964d\u4f4e\u5e9f\u6c34\u4e2d\u7684\u5c3f\u7d20\u542b\u91cf\u3002\u8fd9\u9879\u5de5\u4f5c\u4e3a\u5f00\u53d1\u5177\u6709\u63d0\u9ad8\u6d3b\u6027\u548c\u7a33\u5b9a\u6027\u7684UORs\u66ff\u4ee3\u7535\u50ac\u5316\u5242\u5f00\u8f9f\u4e86\u65b0\u7684\u9014\u5f84\u3002<\/p>\n

\u7b2c\u4e00\u4f5c\u8005\uff1aShi-Kui Geng\uff0c \u90d1\u5c27\uff0c \u674e\u5584\u9752<\/p>\n

\u901a\u8baf\u4f5c\u8005\uff1a\u9648\u5e73\u3001\u5218\u5e86\u534e\u3001\u4e54\u4e16\u748b<\/p>\n

\u901a\u8baf\u5355\u4f4d\uff1a\u5b89\u5fbd\u5927\u5b66\u3001\u4e2d\u56fd\u79d1\u6280\u5927\u5b66\u3001\u963f\u5fb7\u83b1\u5fb7\u5927\u5b66<\/p>\n

\u8bba\u6587doi\uff1a<\/p>\n

https:\/\/doi.org\/10.1038\/s41560-021-00899-2<\/u><\/a><\/p>\n

\u672c\u6587\u7531\u6e29\u534e\u4f9b\u7a3f\u3002<\/p>\n

\u56e2\u961f\u4ecb\u7ecd<\/b><\/strong><\/p>\n

\u4e54\u4e16\u748b\u6559\u6388\uff0c\u73b0\u4efb\u6fb3\u5927\u5229\u4e9a\u963f\u5fb7\u83b1\u5fb7\u5927\u5b66\u5316\u5de5\u4e0e\u6750\u6599\u5b66\u9662\u7eb3\u7c73\u6280\u672f\u9996\u5e2d\u6559\u6388\uff0c\u6842\u51a0\u6559\u6388, \u80fd\u6e90\u4e0e\u50ac\u5316\u6750\u6599\u4e2d\u5fc3\uff08Centre for Materials in Energy and Catalysis\uff09\u4e3b\u4efb\uff0c\u4e3b\u8981\u4ece\u4e8b\u65b0\u80fd\u6e90\u6280\u672f\u7eb3\u7c73\u6750\u6599\u9886\u57df\u7684\u7814\u7a76\uff0c\u5305\u62ec\u7535\u6c60\u3001\u7535\u50ac\u5316\u3001\u5149\u50ac\u5316\u7b49\u3002\u4f5c\u4e3a\u901a\u8baf\u8054\u7cfb\u4eba\uff0c\u5728 Nature\u3001Nature Energy\u3001Nature Chemistry\u3001 Nature Communications\u3001Journal of American Chemical Society\u3001Angewandte Chemie-International Edition\u3001Advanced Materials \u7b49\u56fd\u9645\u9876\u7ea7\u671f\u520a\u53d1\u8868\u5b66\u672f\u8bba\u6587\u8d85\u8fc7450\u7bc7\uff0c\u5f15\u7528\u8d85\u8fc783500\u6b21\uff0ch\u6307\u6570\u4e3a151\u3002\u4e54\u4e16\u748b\u6559\u6388\u5df2\u83b7\u5f97\u591a\u9879\u91cd\u8981\u5956\u52b1\u4e0e\u8363\u8a89\uff0c\u5305\u62ec2017\u5e74\u6fb3\u5927\u5229\u4e9a\u7814\u7a76\u7406\u4e8b\u4f1a\u6842\u51a0\u5b66\u8005\uff08ARC Australian Laureate Fellow\uff09\u30012016\u5e74\u57c3\u514b\u68ee\u7f8e\u5b5a\u5956\u30012013\u5e74\u7f8e\u56fd\u5316\u5b66\u5b66\u4f1a\u80fd\u6e90\u4e0e\u71c3\u6599\u90e8\u65b0\u5174\u7814\u7a76\u8005\u5956\u4ee5\u53ca\u6fb3\u5927\u5229\u4e9a\u7814\u7a76\u7406\u4e8b\u4f1a\u6770\u51fa\u7814\u7a76\u8005\u5956\uff08DORA\uff09\u3002\u4e54\u6559\u6388\u662f\u56fd\u9645\u5316\u5b66\u5de5\u7a0b\u5e08\u5b66\u4f1a\u4f1a\u58eb\u3001\u6fb3\u5927\u5229\u4e9a\u7687\u5bb6\u5316\u5b66\u4f1a\u4f1a\u58eb\u3001\u82f1\u56fd\u7687\u5bb6\u5316\u5b66\u4f1a\u4f1a\u58eb\u7b49\u3002\u540c\u65f6\uff0c\u4ed6\u62c5\u4efb\u56fd\u9645\u520a\u7269\u82f1\u56fd\u7687\u5bb6\u5316\u5b66\u4f1a\u5fd7 Journal of Materials Chemistry A\u526f\u4e3b\u7f16\uff0c\u4e5f\u662f\u79d1\u777f\u552f\u5b89\u5316\u5b66\u53ca\u6750\u6599\u79d1\u5b66\u4e24\u4e2a\u9886\u57df\u7684\u9ad8\u88ab\u5f15\u79d1\u5b66\u5bb6\u3002<\/p>\n

\u90d1\u5c27\u526f\u6559\u6388\uff0c2014\u5e74\u535a\u58eb\u6bd5\u4e1a\u4e8e\u6606\u58eb\u5170\u5927\u5b66\uff0c\u76ee\u524d\u4e3a\u963f\u5fb7\u83b1\u5fb7\u5927\u5b66\u5316\u5de5\u4e0e\u6750\u6599\u5b66\u9662\u526f\u6559\u6388\u3002\u4e3b\u8981\u7814\u7a76\u65b9\u5411\u4e3a\u7535\u5316\u5b66\u80fd\u6e90\u8f6c\u5316\uff0c\u5305\u62ec\u7535\u70bc\u5316\uff08electrocatalytic refinery\uff09\uff0c\u6c34\u88c2\u89e3\uff0c\u4e8c\u6c27\u5316\u78b3\u8fd8\u539f\u7b49\u3002 \u7740\u91cd\u91c7\u7528\u7406\u8bba\u8ba1\u7b97\u4e0e\u5b9e\u9a8c\u76f8\u7ed3\u5408\u7684\u624b\u6bb5\u8fdb\u884c\u9ad8\u6027\u80fd\u50ac\u5316\u5242\u7684\u8bbe\u8ba1\u4e0e\u5f00\u53d1\u3002\u76ee\u524d\u4f5c\u4e3a\u7b2c\u4e00\u4f5c\u8005\u548c\u901a\u8baf\u4f5c\u8005\u5df2\u5728Nature Energy (2\u7bc7), Nature Chemistry, Nature Commun. (2\u7bc7), JACS (8\u7bc7), Angew. Chem. (4\u7bc7), Adv. Mater. (4\u7bc7)\uff0cCHEM(4\u7bc7), Chem. Rev., Chem. Soc. Rev., \u7b49\u6742\u5fd7\u4e0a\u53d1\u8868\u8bba\u658760\u4f59\u7bc7\uff0c\u8bba\u6587\u603b\u6570\u4e3a120\u4f59\u7bc7 (\u5305\u62ec43\u7bc7ESI\u9ad8\u88ab\u5f15\u6587\u7ae0)\uff0c\u5f15\u7528\u8d85\u8fc725,000\u6b21\uff0cH\u56e0\u5b50\u4e3a63\u3002\u83b7\u5f97\u6fb3\u5927\u5229\u4e9a\u7814\u7a76\u7406\u4e8b\u4f1a(ARC) Future Fellowship, Discovery Project\uff0cDECRA\u9879\u76ee\u5171\u8ba1270\u4f59\u4e07\u6fb3\u5143\u7684\u8d44\u52a9\u3002\u4ed6\u4e5f\u662f\u79d1\u777f\u552f\u5b89\u5316\u5b66\u9886\u57df\u7684\u9ad8\u88ab\u5f15\u79d1\u5b66\u5bb6\u3002<\/p>\n

\u8be5\u56e2\u961f\u76ee\u524d\u62db\u52df2-4\u540d\u535a\u58eb\u751f<\/b><\/strong><\/p>\n

\u7814\u7a76\u65b9\u5411<\/b><\/strong><\/p>\n

\u5148\u8fdb\u7535\u50ac\u5316\u53cd\u5e94\u53ca\u673a\u7406\u63a2\u7d22\uff0c\u901a\u8fc7\u6750\u6599\u8bbe\u8ba1\uff0c\u539f\u4f4d\u5149\u8c31\uff0c\u7406\u8bba\u8ba1\u7b97\u7b49\u65b9\u6cd5\u8fdb\u884c\u7535\u50ac\u5316\u6750\u6599\u7684\u5f00\u53d1\uff0c\u5305\u62ec\u4f46\u4e0d\u9650\u4e8e<\/p>\n