{"id":132740,"date":"2018-04-08T14:00:39","date_gmt":"2018-04-08T06:00:39","guid":{"rendered":"\/\/m.iemloyee.com\/?p=132740"},"modified":"2018-04-05T16:53:23","modified_gmt":"2018-04-05T08:53:23","slug":"%e5%8c%85%e4%bf%a1%e5%92%8c%e5%9b%a2%e9%98%9fees-%e9%85%8d%e4%bd%8d%e4%b8%8d%e9%a5%b1%e5%92%8cni-n%e6%b4%bb%e6%80%a7%e4%bd%8d%e9%ab%98%e6%95%88%e5%82%ac%e5%8c%96co2%e7%94%b5%e5%8c%96%e5%ad%a6","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=132740","title":{"rendered":"\u5305\u4fe1\u548c\u56e2\u961fEES: \u914d\u4f4d\u4e0d\u9971\u548cNi-N\u6d3b\u6027\u4f4d\u9ad8\u6548\u50ac\u5316CO2\u7535\u5316\u5b66\u8fd8\u539f"},"content":{"rendered":"

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

\u4e8c\u6c27\u5316\u78b3\u7535\u5316\u5b66\u8fd8\u539f\u53cd\u5e94\uff08CO2<\/sub>RR\uff09\u53ef\u540c\u65f6\u5b9e\u73b0\u95f4\u6b47\u6027\u53ef\u518d\u751f\u7535\u529b\u7684\u50a8\u5b58\u548c\u6e29\u5ba4\u6c14\u4f53CO2<\/sub>\u7684\u8f6c\u5316\u5229\u7528\uff0c\u5229\u4e8e\u6784\u5efa\u53ef\u6301\u7eed\u7684\u78b3\u8d44\u6e90\u5faa\u73af\u5229\u7528\u7f51\u7edc\u3002\u8fd1\u5e74\u6765\u7684\u7814\u7a76\u8868\u660e\uff0c\u8fc7\u6e21\u91d1\u5c5e-\u6c2e-\u78b3\u590d\u5408\u6750\u6599\u53ef\u5c06CO2<\/sub>\u7535\u8fd8\u539f\u751f\u6210CO\uff0c\u4f46\u968f\u7740\u8fc7\u7535\u52bf\u589e\u52a0\uff0c\u7ade\u4e89\u6027\u7684\u6790\u6c22\u53cd\u5e94(HER)\u7535\u6d41\u6025\u5267\u589e\u5927\uff0c\u9020\u6210CO\u6cd5\u62c9\u7b2c\u6548\u7387\u8fc5\u901f\u4e0b\u964d\uff0c\u5f88\u96be\u83b7\u5f97\u9ad8\u7684CO\u5206\u7535\u6d41\u5bc6\u5ea6\u3002\u56e0\u6b64\u540c\u65f6\u83b7\u5f97\u9ad8\u7684CO2<\/sub>RR\u7535\u6d41\u5bc6\u5ea6\u548c\u6cd5\u62c9\u7b2c\u6548\u7387\u662f\u8fc7\u6e21\u91d1\u5c5e-\u6c2e-\u78b3\u590d\u5408\u6750\u6599\u9762\u4e34\u7684\u91cd\u8981\u6311\u6218\uff0c\u8fd9\u4e5f\u662fCO2<\/sub>RR\u672a\u6765\u5b9e\u9645\u5e94\u7528\u5728\u9ad8\u53cd\u5e94\u901f\u7387\u548c\u9009\u62e9\u6027\u65b9\u9762\u7684\u5fc5\u7136\u9700\u6c42\u3002<\/p>\n

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

\u8fd1\u671f\uff0c\u5927\u8fde\u5316\u7269\u6240\u5305\u4fe1\u548c\u9662\u58eb\u548c\u6c6a\u56fd\u96c4\u7814\u7a76\u5458<\/strong>\uff08\u5171\u540c\u901a\u8baf\u4f5c\u8005\uff09\u5728Energy &Environmental Science\u4e0a\u53d1\u8868\u9898\u4e3a\u201cCoordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2<\/sub> electroreduction\u201d\u7684\u6587\u7ae0(\u7b2c\u4e00\u4f5c\u8005\u960e\u7a0b\u7a0b\u535a\u58eb\u751f\u548c\u674e\u660a\u535a\u535a\u58eb)\uff0c\u9610\u8ff0\u4e86\u914d\u4f4d\u4e0d\u9971\u548c\u7684Ni-N\u6d3b\u6027\u4f4d\u5728CO2<\/sub>\u9ad8\u6548\u7535\u50ac\u5316\u8fd8\u539f\u4e2d\u7684\u5e94\u7528\u3002\u8be5\u7814\u7a76\u901a\u8fc7\u70ed\u89e3\u950c\/\u954d\u53cc\u91d1\u5c5e\u6cb8\u77f3\u54aa\u5511\u7c7b\u9aa8\u67b6\u6750\u6599(ZIF-8), \u6210\u529f\u5236\u5907\u51fa\u914d\u4f4d\u4e0d\u9971\u548cNi-N\u4f4d\u63ba\u6742\u7684\u591a\u5b54\u78b3\u6750\u6599\uff0c\u5176\u4e2d\u5355\u5206\u6563\u7684Ni\u7269\u79cd\u8d1f\u8f7d\u91cf\u6700\u9ad8\u53ef\u8fbe5.44 wt\uff05\u3002\u5728\u8be5Ni-N\u50ac\u5316\u5242\u4e0a\uff0cCO\u6cd5\u62c9\u7b2c\u6548\u7387\u5728-0.53V\u301c-1.03 V (vs. RHE)\u5bbd\u7535\u52bf\u533a\u95f4\u5185\u7ef4\u6301\u572892.0%\u301c98.0%\u4e4b\u95f4\uff0cCO\u7535\u6d41\u5bc6\u5ea6\u968f\u8fc7\u7535\u52bf\u589e\u52a0\u800c\u589e\u52a0\uff0c\u5728-1.03 V (vs. RHE)\u8fbe\u523071.5\u00b12.9 mA cm-2<\/sup>\u3002\u8868\u5f81\u7ed3\u679c\u548c\u5bf9\u6bd4\u5b9e\u9a8c\u8868\u660e\u914d\u4f4d\u4e0d\u9971\u548c\u7684Ni-N\u4e3a\u6d3b\u6027\u4f4d\u70b9\uff1b\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\u8ba1\u7b97\u8fdb\u4e00\u6b65\u63ed\u793a\u5728NiN2<\/sub>V2<\/sub> (V\u8868\u793a\u7a7a\u4f4d) \u4f4d\u4e0aCO2<\/sub>RR\u6bd4HER\u66f4\u5bb9\u6613\u53d1\u751f\uff0c\u63a8\u6d4bNiN2<\/sub>V2<\/sub>\u53ef\u80fd\u662fCO2<\/sub>RR\u7684\u6d3b\u6027\u4f4d\u3002\u56e0\u6b64\uff0c\u9ad8\u8f7d\u91cf\u914d\u4f4d\u4e0d\u9971\u548cNi-N\u6d3b\u6027\u4f4d\u540c\u65f6\u5b9e\u73b0\u4e86CO2<\/sub>RR\u7684\u9ad8\u7535\u6d41\u5bc6\u5ea6\u548c\u6cd5\u62c9\u7b2c\u6548\u7387\u3002<\/p>\n

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

\u56fe1 \u56fe\u6458\u8981<\/strong><\/p>\n

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

\u56fe<\/strong>2 <\/strong>\u50ac\u5316\u5242\u5236\u5907\u6d41\u7a0b\u53ca\u7535\u955c\u56fe<\/strong><\/p>\n

\"\"<\/p>\n

\uff08a\uff09C-Znx<\/sub>Niy<\/sub> ZIF-8\u7684\u5236\u5907\u6d41\u7a0b\u56fe\uff1b<\/p>\n

\uff08b\uff09C-Zn1<\/sub>Ni4<\/sub> ZIF-8\u7684\u4f4e\u5206\u8fa8\u7387HAADF-STEM\u56fe\u50cf\u548cC\uff0cN\uff0cNi\uff0cZn \u7684EDS\u56fe\u50cf\uff1b<\/p>\n

\uff08c\uff09C-Zn1<\/sub>Ni4<\/sub> ZIF-8\u7684HRTEM\u56fe\u50cf\uff1b<\/p>\n

\uff08d\uff09C-Zn1<\/sub>Ni4<\/sub> ZIF-8\u7684\u9ad8\u5206\u8fa8\u7387HAADF-STEM\u56fe\u50cf\uff1b<\/p>\n

\u56fe<\/strong>3<\/strong> C-Znx<\/sub>Niy<\/sub> ZIF-8<\/strong>\u7ed3\u6784\u4e0e\u7ec4\u6210\u8868\u5f81<\/strong><\/p>\n

\"\"<\/p>\n

\"\"<\/p>\n

\uff08a\uff09XRD\u8c31\u56fe;<\/p>\n

\uff08b\uff09C-Znx<\/sub>Niy<\/sub> ZIF-8\u548cNiPc\u7684Ni 2p\u9ad8\u5206\u8fa8XPS\u8c31\u56fe\uff1b<\/p>\n

\uff08c\uff09C-Znx<\/sub>Niy<\/sub> ZIF-8\u548c\u76f8\u5e94\u6807\u6837\u7684Ni-K\u8fb9XANES\u8c31\u56fe\uff1b<\/p>\n

\uff08d\uff09C-Znx<\/sub>Niy<\/sub> ZIF-8\u548c\u76f8\u5e94\u6807\u6837\u7684Ni-K\u8fb9EXAFS\u8c31\u56fe\uff08\u865a\u7ebf\u8868\u793a\u62df\u5408\u7ed3\u679c\uff09\uff1b<\/p>\n

\u56fe<\/strong>4<\/strong> CO2<\/sub>RR<\/strong>\u6027\u80fd\u7ed3\u679c<\/strong><\/p>\n

\"\"<\/p>\n

\"\"<\/p>\n

\uff08a\uff09CO\u6cd5\u62c9\u7b2c\u6548\u7387\u548c\uff08b\uff09CO\u5206\u7535\u6d41\u5bc6\u5ea6\u968f\u7535\u52bf\u7684\u53d8\u5316\u8d8b\u52bf\uff1b\u6d4b\u8bd5\u6761\u4ef6\uff1aC-Znx<\/sub>Ny<\/sub> ZIF-8\u8f7d\u91cf\u4e3a2.0F0.1mg cm-2<\/sup>\uff0cNiPc\u8f7d\u91cf\u4e3a1.06 mg cm-2<\/sup>\uff0cCO2<\/sub>\u9971\u548c\u76841 M KHCO3<\/sub>\u6eb6\u6db2\u3002<\/p>\n

\uff08c\uff09CO\u6cd5\u62c9\u7b2c\u6548\u7387\u548c\uff08d\uff09\u50ac\u5316\u5242\u8f6c\u5316\u9891\u7387\u503c\uff08TOF\uff09\u968f\u7535\u52bf\u7684\u53d8\u5316\u8d8b\u52bf\uff1b\u6d4b\u8bd5\u6761\u4ef6\uff1aC-Zn1<\/sub>Ni4<\/sub> ZIF-8\u8f7d\u91cf\u4e3a0.088 mg cm-2<\/sup>\uff0cC-Zn1<\/sub>Ni1<\/sub> ZIF-8\u8f7d\u91cf\u4e3a0.226 mg cm-2<\/sup>\uff0cCO2<\/sub>\u9971\u548c\u76840.5 M KHCO3<\/sub>\u6eb6\u6db2\u3002<\/p>\n

\u56fe<\/strong>5 <\/strong>\u50ac\u5316\u5242<\/strong>CO2<\/sub>RR<\/strong>\u7a33\u5b9a\u6027\u6d4b\u8bd5\u7ed3\u679c\u53ca\u53cd\u5e94\u6027\u80fd\u4e0e<\/strong>Ni<\/strong>\u8f7d\u91cf\u7684\u5173\u7cfb\u56fe<\/strong><\/p>\n

\"\"<\/p>\n

\uff08a\uff09\u5728-0.63 V (vs. RHE)\u65f6C-Zn1<\/sub>Ni ZIF-8\u7684\u7a33\u5b9a\u6027\u6d4b\u8bd5\u7ed3\u679c\uff1b<\/p>\n

\uff08b\uff09\u5728-0.83 V(vs. RHE)\u65f6\uff0c\u5177\u6709\u4e0d\u540cNi\u8f7d\u91cf\u7684\u50ac\u5316\u5242\u4e0aCO\u5206\u7535\u6d41\u5bc6\u5ea6\u4e0eNi\u542b\u91cf\u7684\u5173\u7cfb\u56fe\uff1b\u6d4b\u8bd5\u6761\u4ef6\uff1a\u50ac\u5316\u5242\u8f7d\u91cf\u4e3a2.0\u8f7d0.1mg cm-2<\/sup>\uff0cCO2<\/sub>\u9971\u548c\u76841 M KHCO3<\/sub>\u6eb6\u6db2\u3002<\/p>\n

\u56fe<\/strong>6 DFT<\/strong>\u8ba1\u7b97<\/strong><\/p>\n

\"\"<\/p>\n

\"\"<\/p>\n

\uff08a\uff09\u5177\u6709\u4e0d\u540cN\u539f\u5b50\u914d\u4f4d\u6570\u7684Ni-N\u7ed3\u6784\u7684\u4f18\u5316\u7ed3\u6784\u56fe\uff1b<\/p>\n

\uff08b-c\uff09\u57280 V\u4e0b\uff0c\u4e0d\u540cNi-N\u7ed3\u6784\u4e2dNi\u4f4d\u70b9\u4e0a\u7684CO2<\/sub>RR\uff08b\uff09\u548cHER\uff08c\uff09\u53cd\u5e94\u8def\u5f84\u7684\u81ea\u7531\u80fd\u53d8\u5316\u56fe\uff0c\u5b9e\u7ebf\u548c\u865a\u7ebf\u5206\u522b\u4ee3\u8868\u5f15\u5165\u9690\u6027\u548c\u663e\u6027\u6eb6\u5242\u5316\u6548\u5e94\u6821\u6b63\u7684\u8ba1\u7b97\u7ed3\u679c\uff1b\u9876\u90e8\u4e3a\u4f18\u5316\u540e\u7684* COOH\u548c* H\u4e2d\u95f4\u4f53\u7684\u5438\u9644\u6784\u578b\u56fe\uff1b\u63d2\u56fe\u4e3a\u5728NiN2<\/sub>V2<\/sub>\u4f4d\u70b9\u5468\u56f4\u6dfb\u52a0\u4e00\u4e2a\u6c34\u5206\u5b50\u5c42\u6765\u6a21\u62df\u6eb6\u5242\u5316\u6548\u5e94\u540e *COOH\u548c* H\u4e2d\u95f4\u4f53\u7684\u5438\u9644\u6784\u578b\u3002\u767d\u8272\uff0c\u7070\u8272\uff0c\u7ea2\u8272\uff0c\u84dd\u8272\uff0c\u7d2b\u8272\u7684\u7403\u5206\u522b\u4ee3\u8868H\uff0cC\uff0cO\uff0cN\uff0cNi\u539f\u5b50\u3002<\/p>\n

\u3010\u5c0f\u7ed3\u3011<\/strong><\/p>\n

\u603b\u7684\u6765\u8bf4\uff0c\u8be5\u7814\u7a76\u8bc1\u660e\u9ad8\u8f7d\u91cf\u914d\u4f4d\u4e0d\u9971\u548cNi-N\u6d3b\u6027\u4f4d\u53ef\u5c06CO2<\/sub>\u9ad8\u9009\u62e9\u6027\u5730\u7535\u50ac\u5316\u8fd8\u539f\u751f\u6210CO\u3002\u5728-0.53 V\u301c-1.03 V\uff08vs. RHE\uff09\u7684\u5bbd\u7535\u52bf\u533a\u95f4\u5185CO\u6cd5\u62c9\u7b2c\u6548\u7387\u7ef4\u6301\u572892.0\uff05\u301c98.0\uff05\u4e4b\u95f4; CO\u5206\u7535\u6d41\u6700\u9ad8\u53ef\u8fbe 71.5\u00b12.9 mA cm-2<\/sup>, \u663e\u793a\u51fa\u4f18\u5f02\u7684CO2<\/sub>\u7535\u50ac\u5316\u8fd8\u539f\u6027\u80fd\u3002\u7406\u8bba\u7ed3\u7b97\u8ba1\u7b97\u7ed3\u679c\u8868\u660e\uff0c\u914d\u4f4d\u4e0d\u9971\u548c\u7684Ni-N\u6d3b\u6027\u4f4d\u5177\u6709\u9ad8\u7684CO2<\/sub>RR\u6d3b\u6027\uff0c\u540c\u65f6\u53ef\u6291\u5236\u7ade\u4e89\u6027\u7684HER\u53cd\u5e94\u3002\u8be5\u50ac\u5316\u5242\u6253\u7834\u4e86\u8fc7\u6e21\u91d1\u5c5e-\u6c2e-\u78b3\u590d\u5408\u6750\u6599\u4e0aCO2<\/sub>RR\u9009\u62e9\u6027\u548c\u53cd\u5e94\u901f\u7387\u7684\u201c\u8df7\u8df7\u677f\u201d\u6548\u5e94\u9650\u5236\uff0c\u5b9e\u73b0\u4e86\u9ad8\u6548\u50ac\u5316CO2<\/sub>RR\u3002<\/p>\n

\u56e2\u961f\u4ecb\u7ecd\uff1a<\/strong><\/p>\n

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

[1] D. F. Gao, H. Zhou, G. X. Wang, J. G. Wang, X. H. Bao, et al., J. Am. Chem. Soc.<\/em>, 2015, 137, 4288.<\/p>\n

[2] Z. Yin, D. F. Gao, G. X. Wang, D. Ma, X. H. Bao, et al., Nano Energy<\/em>, 2016, 27, 35.<\/p>\n

[3] D. F. Gao, H. Zhou, F. Cai, J. G. Wang, G. X. Wang, X. H. Bao, et al., Nano Research<\/em>, 2017, 10, 2181.<\/p>\n

[4] F. Cai, D. F. Gao, G. X. Wang, X. H. Bao, et al., Chem. Sci.<\/em>, 2017, 8, 2569.<\/strong><\/p>\n

[5] D. F. Gao, G. X. Wang, X. H. Bao, ACS Catal.<\/em>, 2018, 8, 1510.<\/strong><\/p>\n

[6] D. F. Gao, Y. Zhang, Z. W. Zhou, F. Yang, G. X. Wang, X. H. Bao, et al., J. Am. Chem. Soc.<\/em>, 2017, 139, 5652.<\/p>\n

[7] H. H. Wu, H. B. Li, G. X. Wang, X. H. Bao, et al., Energy Environ. Sci.<\/em>, 2016, 9, 3736.<\/p>\n

[8] Y. F. Ye, H. B. Li, G. X. Wang, X. H. Bao, et al., ACS Catal.<\/em><\/strong>, 2017, 7, 7638.<\/strong><\/p>\n

[9] Y. F. Ye, F. Cai, G. X. Wang, Y. S. Li, X. H. Bao, et al., Nano Energy<\/em>, 2017, 38, 281.<\/p>\n

[10] C. C. Yan, H. B. Li, G. X. Wang, X. H. Bao, et al., Energy Environ. Sci.<\/em>, 2018, DOI:10.1039\/C8EE00133B.<\/p>\n

\u6587\u732e\u94fe\u63a5<\/strong>\uff1aCoordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2<\/sub> electroreduction<\/a> (Energy & Environmental Science,<\/em> 2018, DOI: 10.1039\/C8EE00133B)<\/p>\n

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