{"id":184940,"date":"2019-09-03T06:30:01","date_gmt":"2019-09-02T22:30:01","guid":{"rendered":"\/\/m.iemloyee.com\/?p=184940"},"modified":"2019-09-02T18:24:56","modified_gmt":"2019-09-02T10:24:56","slug":"%e5%9b%9b%e5%b7%9d%e5%a4%a7%e5%ad%a6j-mater-chem-a%ef%bc%9aau-cu%e5%8a%a9%e5%82%ac%e5%8c%96%e5%89%82%e8%b0%83%e6%8e%a7%e5%85%89%e5%82%ac%e5%8c%96co2rr%e9%80%89%e6%8b%a9%e6%80%a7%e7%9a%84%e5%8f%8d","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=184940","title":{"rendered":"\u56db\u5ddd\u5927\u5b66J Mater Chem A\uff1aAu\/Cu\u52a9\u50ac\u5316\u5242\u8c03\u63a7\u5149\u50ac\u5316CO2RR\u9009\u62e9\u6027\u7684\u53cd\u5e94\u673a\u7406"},"content":{"rendered":"

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

\u8fd1\u65e5\uff0c\u56db\u5ddd\u5927\u5b66\u535a\u58eb\u751f\u674e\u89e3\u5143\uff08\u7b2c\u4e00\u4f5c\u8005\uff09\u5728\u5c91\u671b\u6765\u526f\u7814\u7a76\u5458\u548c\u695a\u82f1\u8c6a\u6559\u6388\uff08\u901a\u8baf\u4f5c\u8005\uff09\u7684\u6307\u5bfc\u4e0b\uff0c\u5728\u56fd\u9645\u9876\u7ea7\u6750\u6599\u671f\u520aJournal of Materials Chemistry A\u4e0a\u53d1\u8868\u4e86\u6587\u7ae0\uff1aCu supported on polymeric carbon nitride for selective CO2<\/sub>\u00a0reduction into CH4<\/sub>: a combined kinetics and thermodynamics investigation\uff08DOI: 10.1039\/c9ta05112k\uff09\u3002\u5229\u7528\u6df1\u5165\u7684DFT\u6a21\u62df\u8ba1\u7b97\u5bf9Cu\u8d1f\u8f7d\u6c2e\u5316\u78b3\u5149\u50ac\u5316\u5bf9CO2<\/sub>\u8fd8\u539f\u7684\u9009\u62e9\u6027\u53ca\u4ea7\u7269\u5206\u5e03\u8fdb\u884c\u4e86\u7814\u7a76\u3002<\/p>\n

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

\u52a9\u50ac\u5316\u5242\/\u534a\u5bfc\u4f53\u7684\u5408\u6210\u6709\u5229\u4e8e\u63d0\u9ad8\u50ac\u5316\u53cd\u5e94\u7684\u9009\u62e9\u6027\uff0c\u91d1\u5c5e\u57fa\u52a9\u50ac\u5316\u5242\u5df2\u88ab\u5e7f\u6cdb\u5e94\u7528\u4e8e\u5149\u50ac\u5316\u4e8c\u6c27\u5316\u78b3\u8fd8\u539f\u53cd\u5e94\uff08CO2<\/sub>RR\uff09\u3002\u7136\u800c\uff0c\u5373\u4f7f\u5728\u76f8\u540c\u7684\u52a9\u50ac\u5316\u5242\/\u534a\u5bfc\u4f53\u5149\u50ac\u5316\u4f53\u7cfb\u4e2d\uff0c\u4ea7\u7269\u7684\u79cd\u7c7b\u548c\u4ea7\u7387\u4e5f\u5b58\u5728\u8f83\u5927\u7684\u5dee\u5f02\uff0c\u8fd9\u9700\u8981\u5bf9\u53cd\u5e94\u673a\u7406\u548c\u4ea7\u7269\u5206\u5e03\u8fdb\u884c\u8be6\u7ec6\u7684\u7814\u7a76\u3002\u672c\u6587\u4e2d\uff0c\u901a\u8fc7\u63d0\u4f9b\u52a8\u529b\u5b66\u8bc1\u636e\u8868\u660e\uff0cCu\u8d1f\u8f7d\u78b3\u5316\u6c2e\uff08Cu \/ CN\uff09\u53ef\u5c06CO2<\/sub>\u9009\u62e9\u6027\u8fd8\u539f\u4e3aCH4<\/sub>\uff0cAu\u8d1f\u8f7d\u78b3\u5316\u6c2e\uff08Au \/ CN\uff09\u4ea7\u7269\u4e3aCO\u548cCH3<\/sub>OH\u3002\u6b64\u5916\uff0c\u63ed\u793a\u4e86CH3<\/sub>OH\u7684\u5438\u9644\/\u89e3\u5438\u70ed\u529b\u5b66\u884c\u4e3a\u662f\u51b3\u5b9a\u4ea7\u7269\u5206\u5e03\u7684\u5173\u952e\u56e0\u7d20\u3002\u901a\u8fc7\u5728\u88ab\u5438\u9644\u7684CH3<\/sub>OH \u4e0eCu \/ CN\u754c\u9762\u5904\u5efa\u7acb\u4e8c\u5143\u7535\u5b50\u4f20\u8f93\u901a\u9053\uff0c\u5b9e\u73b0CH3<\/sub>OH\u7684\u6d3b\u6027\uff0c\u4f7f\u5f97CO2<\/sub>\u5b8c\u5168\u8fd8\u539f\u4e3aCH4<\/sub>\u3002\u7531\u4e8e\u5728\u539f\u5b50\u6c34\u5e73\u4e0a\u7684\u52a8\u529b\u5b66\u548c\u70ed\u529b\u5b66\u7814\u7a76\uff0c\u8fd9\u9879\u5de5\u4f5c\u53ef\u4ee5\u4e3a\u9009\u62e9\u6027CO2<\/sub>RR\u7684\u52a9\u50ac\u5316\u5242\/\u534a\u5bfc\u4f53\u7cbe\u7ec6\u5316\u5b9a\u5236\u63d0\u4f9b\u8bbe\u8ba1\u65b9\u6848\u3002<\/p>\n

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

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

Fig. 1<\/b><\/strong>\u00a0Catalyst properties: calculated absorption spectra (a); total density of states (DOS, (b)); projected DOS (c); electronic localization function (ELF) and charge density difference result for Au\/CN (d and e) and Cu\/CN (f and g). Blue, grey, gold and green spheres refer to C, N, Au and Cu atoms, respectively. Electron depletion is given in yellow and accumulation is given in blue. The isosurfaces of e and g are both set to 0.006 eV\u00c5-3<\/sup>. Positive values of q<\/i><\/em>\u00a0depict electron depletion.<\/p>\n

Cu \/ CN\u548c Au \/ CN\u51cf\u5c11\u7684\u5e26\u9699\u5bbd\u5ea6\uff0c\u4e14Cu \/ CN\u7684\u63a5\u89e6\u754c\u9762\u6bd4Au \/ CN\u7684\u63a5\u89e6\u754c\u9762\u5177\u6709\u66f4\u7262\u56fa\u7684\u5171\u4ef7\u952e\u548c\u66f4\u5f3a\u7684\u7535\u5b50\u76f8\u4e92\u4f5c\u7528\u3002<\/p>\n

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

Scheme 1<\/b><\/strong>\u00a0Possible reaction pathways for the photocatalytic CO2<\/sub>\u00a0reduction reaction to form C1 products. Each reduction reaction requires H+<\/sup>\u00a0and e–<\/sup>\u00a0to proceed, which are not shown in the scheme. The * symbol indicates that the corresponding intermediate is adsorbed on the catalyst surface.<\/p>\n

CO2<\/sub>RR\u53cd\u5e94\u9014\u5f84\u7684\u4e2d\u95f4\u4ea7\u7269\u7684\u8131\u9644\u548c\u8fd8\u539f\u53cd\u5e94\u4e4b\u95f4\u5b58\u5728\u7ade\u4e89\uff0c\u5bfc\u81f4\u4ea7\u7269\u5206\u5e03\u4e0d\u660e\u786e\uff0c\u5f71\u54cd\u53cd\u5e94\u9009\u62e9\u6027\u3002<\/p>\n

\"\"<\/p>\n

Fig. 2<\/strong> Reaction kinetics: calculated reaction pathways using the climbing image nudged elastic band (CI-NEB) method for the photocatalytic CO2<\/sub>RR on Au\/CN (a) and Cu\/CN (b).<\/p>\n

CO2<\/sub>\u52a0\u6c22\u53cd\u5e94\u4e3aCO2<\/sub>RR\u7684\u901f\u63a7\u6b65\u9aa4\u3002Au \/ CN\u4e0a\uff0cCO2<\/sub>\u503e\u5411\u8fd8\u539f\u4e3aCO\u548cCH3<\/sub>OH\uff1bCu \/ CN\u4e0a\uff0cCO2<\/sub>\u52a0\u6c22\u540e\u9009\u62e9\u6027\u751f\u6210CH4<\/sub>\u3002<\/p>\n

\"\"<\/p>\n

Fig. 3<\/b><\/strong>\u00a0Adsorption\/desorption thermodynamics: calculated Ab Initio<\/i><\/em>\u00a0molecular dynamics (AIMD) results for CO*Au\/CN (a), CH3<\/sub>OH*Au\/CN (b) and CH3<\/sub>OH*Cu\/CN. Blue, grey, gold, green, red and pink spheres depict C, N, Au, Cu, O and H atoms, respectively<\/p>\n

\u901a\u8fc7\u5e38\u6e29\u5e38\u538b\u4e0b\u7684\u70ed\u529b\u5b66\u8ba1\u7b97\uff0c\u8fdb\u4e00\u6b65\u8bc1\u660e\u5b9e\u9645\u60c5\u51b5\u4e0bCO2<\/sub>RR\u5728Au \/ CN\u548cCu \/ CN\u7684\u53cd\u5e94\u9014\u5f84\u3002CO\u548cCH3<\/sub>OH\u5728Au \/ CN\u4e0a\u8131\u9644\u5e76\u6210\u4e3a\u7ec8\u4ea7\u7269\uff0cCH3<\/sub>OH\u5728Cu \/ CN\u8868\u9762\u5438\u9644\u6d3b\u5316\u4e0a\u88ab\u8fdb\u4e00\u6b65\u8fd8\u539f\u4e3aCH4<\/sub>\u3002<\/p>\n

\"\"<\/p>\n

Fig. 4<\/b><\/strong>\u00a0Electronic properties of adsorbed complexes: calculated projected density of states (DOS) for CH3OH*Au\/CN (a) and CH3<\/sub>OH*Cu\/CN(b); electronic localization function (ELF) and charge density difference results CH3<\/sub>OH*Au\/CN (c and d) and CH3<\/sub>OH*Cu\/CN (e and f). Blue, grey, gold and green spheres refer to C, N, Au and Cu atoms, respectively. Electron depletion is shown in yellow and accumulation is shown in blue. The isosurfaces (d and f) are both set to 0.01 eV \u00c5–<\/sup>3<\/sup>. Positive and negative q<\/i><\/em>\u00a0values depict electron depletion and accumulation correspondingly.<\/p>\n

\u6001\u5bc6\u5ea6\u8ba1\u7b97\u4e2d\uff0cCH3<\/sub>OH*Cu \/ CN\u4e3b\u5cf0\u660e\u663e\u91cd\u53e0\uff0cCH3<\/sub>OH\u4e0eCu\/CN\u8868\u9762\u5b58\u5728\u5f3a\u5171\u4ef7\u3002\u7535\u5b50\u5c40\u57df\u51fd\u6570\u548c\u7535\u8377\u5bc6\u5ea6\u53ef\u76f4\u89c2\u770b\u5230\uff0cCH3<\/sub>OH*Cu \/ CN\u5f62\u6210\u4e86C-Cu\u548cO-N\u952e\uff0c\u5efa\u7acb\u4e86\u7535\u5b50\u4f20\u8f93\u7684\u4e8c\u5143\u901a\u9053\u3002\u56e0\u6b64\uff0cCH3<\/sub>OH\u5728Cu \/ CN\u88ab\u8fdb\u4e00\u6b65\u8fd8\u539f\u4e3aCH4<\/sub>\u3002<\/p>\n

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

\"\"<\/p>\n

Fig. 5<\/b><\/strong>\u00a0The illustration of design schemes for the understanding of the\u00a0selective CO2<\/sub>RR on Cu\/CN.<\/p>\n

\u7efc\u4e0a\u6240\u8ff0\uff0cAu \/ CN\u548cCu \/ CN\u4f5c\u4e3a\u5178\u578b\u7684\u52a9\u50ac\u5316\u5242\/\u534a\u5bfc\u4f53\u4f53\u7cfb\uff0c\u4ee5\u7814\u7a76\u5149\u50ac\u5316CO2<\/sub>RR\u7684\u9009\u62e9\u6027\u3002\u901a\u8fc7\u5e7f\u6cdb\u7684\u7406\u8bba\u8ba1\u7b97\uff0c\u5bf9\u50ac\u5316\u5242\u6027\u8d28\uff0c\u53cd\u5e94\u52a8\u529b\u5b66\u548c\u5438\u9644\/\u89e3\u5438\u70ed\u529b\u5b66\u8fdb\u884c\u4e86\u5168\u9762\u7684\u7814\u7a76\u3002\u7ed3\u679c\u8868\u660e\uff0c\u4e0eAu\u539f\u5b50\u76f8\u6bd4\uff0cCu\u539f\u5b50\u4e0e\u76f8\u90bbN\u539f\u5b50\u4e4b\u95f4\u7684\u7535\u5b50\u76f8\u4e92\u4f5c\u7528\u660e\u663e\u589e\u5f3a\uff0c\u4e3a\u9009\u62e9\u6027CO2<\/sub>RR\u63d0\u4f9b\u4e86\u53cd\u5e94\u4f4d\u70b9\u3002\u52a8\u529b\u5b66\u8ba1\u7b97\u8fdb\u4e00\u6b65\u8bc1\u5b9e\uff0cCu \/ CN\u5bf9CH4<\/sub>\u7684\u9009\u62e9\u6027\u6709\u660e\u663e\u63d0\u5347\uff0c\u800cAu \/ CN\u9009\u62e9\u6027\u8f83\u5dee\u751f\u6210CO\u548cCH3<\/sub>OH\u3002CH3<\/sub>OH\u4e0eCu\/CN\u754c\u9762\u7684\u4e8c\u5143\u7535\u5b50\u901a\u9053\u663e\u8457\u4fc3\u8fdb\u4e86CH3<\/sub>OH\u5206\u5b50\u7684\u5438\u9644\u6d3b\u5316\uff0c\u4f7fCH3<\/sub>OH\u8fdb\u4e00\u6b65\u8fd8\u539f\u4e3aCH4<\/sub>\uff0c\u63d0\u9ad8\u9009\u62e9\u6027\u3002\u672c\u7814\u7a76\u4e3a\u5f00\u53d1\u9009\u62e9\u6027CO2<\/sub>\u51cf\u6392\u7684\u52a9\u50ac\u5316\u5242\/\u534a\u5bfc\u4f53\u5149\u50ac\u5316\u7cfb\u7edf\u63d0\u4f9b\u4e86\u4e00\u79cd\u65b0\u7684\u89c6\u89d2\u3002<\/p>\n

\u3010\u56e2\u961f\u4ecb\u7ecd<\/span>\u3011<\/span><\/strong><\/p>\n

\u535a\u58eb\u751f\u674e\u89e3\u5143\uff0c\u7537\uff0c1991\u5e74\u51fa\u751f\uff0c\u91cd\u5e86\u4eba\u3002\u4e8e2014\u5e74\u5728\u56db\u5ddd\u5927\u5b66\u83b7\u73af\u5883\u5de5\u7a0b\u5b66\u58eb\u5b66\u4f4d\uff0c2015\u5e74\u81f3\u4eca\u5728\u56db\u5ddd\u5927\u5b66\u653b\u8bfb\u73af\u5883\u5de5\u7a0b\u535a\u58eb\u5b66\u4f4d\uff0c\u4e3b\u8981\u7814\u7a76\u65b9\u5411\u4e3a\u7b2c\u4e00\u6027\u539f\u7406\u8ba1\u7b97\u4e0e\u5149\u50ac\u5316\u5b9e\u9a8c\u6280\u672f\u7684\u7ed3\u5408\u7814\u7a76\uff0c\u591a\u6b21\u7ec4\u7ec7\u514d\u8d39\u8ba1\u7b97\u6a21\u62df\u57f9\u8bad\u3002\u653b\u8bfb\u7814\u7a76\u751f\u4ee5\u6765\uff0c\u4ee5\u7b2c\u4e00\u4f5c\u8005\u8eab\u4efd\u53d1\u8868SCI\u8bba\u658712\u7bc7\uff0c\u5305\u62ecACS Catalysis, Journal of Materials Chemistry A, Applied Catalysis B: Environmental\u548cACS Applied Materials & Interfaces\u7b49\u77e5\u540d\u671f\u520a\uff0c\u5408\u4f5c\u53d1\u8868\u8bba\u658723\u7bc7\u300213\u7bc7\u5165\u9009ESI\u9ad8\u88ab\u5f15\u8bba\u6587\uff08\u542b4\u7bc7ESI\u70ed\u70b9\u8bba\u6587\uff09\uff0cSCI\u4ed6\u5f15>700\u6b21\uff0cH-index=15\u3002\u83b7\u7b2c\u4e5d\u5c4a\u5168\u56fd\u73af\u5883\u5316\u5b66\u5927\u4f1a\u4f18\u79c0\u53e3\u5934\u62a5\u544a\u5956\uff0c\u56db\u5ddd\u5927\u5b66\u4f18\u79c0\u5b66\u672f\u4e4b\u661f\uff0c\u7814\u7a76\u751f\u56fd\u5bb6\u5956\u5b66\u91d1\uff08\u8fde\u7eed\u4e09\u5e74\uff09\u3001\u7814\u7a76\u751f\u4e00\u7b49\u5956\u5b66\u91d1\uff08\u8fde\u7eed\u56db\u5e74\uff09\u7b49\u8363\u8a89\u3002<\/p>\n

\u5c91\u671b\u6765\u526f\u7814\u7a76\u5458\uff08ResearcherID: E-8768-2012\uff09\uff0c1981\u5e741\u6708\u751f\uff0c\u6e56\u5317\u9ec4\u5188\u4eba\uff0c2012\u5e7412\u6708\u6bd5\u4e1a\u4e8e\u6d59\u6c5f\u5927\u5b66\uff0c\u83b7\u73af\u5883\u5de5\u7a0b\u535a\u58eb\u5b66\u4f4d\uff0c\u53d7\u7559\u5b66\u57fa\u91d1\u59d4\u8d44\u52a9\u5728\u5fb7\u514b\u8428\u65af\u5927\u5b66\u5965\u65af\u6c40\u5206\u6821Graeme Henkelman\u7ec4\u8bbf\u5b66\u4e00\u5e74\u3002\u73b0\u4efb\u56db\u5ddd\u5927\u5b66\u65b0\u80fd\u6e90\u4e0e\u4f4e\u78b3\u6280\u672f\u7814\u7a76\u9662\u526f\u7814\u7a76\u5458\uff0c\u4e3b\u8981\u4ece\u4e8b\u5927\u6c14\u6c61\u67d3\u63a7\u5236\u6280\u672f\u548c\u73af\u5883\u50ac\u5316\u65b9\u9762\u7684\u539f\u5b50\u5c3a\u5ea6\u8ba1\u7b97\u6a21\u62df\u7814\u7a76\u5de5\u4f5c\uff0c\u4e3b\u6301\u56fd\u5bb6\u81ea\u7136\u79d1\u5b66\u57fa\u91d1\u9762\u4e0a\u9879\u76ee\u548c\u9752\u5e74\u57fa\u91d1\u54041\u9879\u3002<\/p>\n

\u3010\u8bfe\u9898\u7ec4\u8fd1\u671f\u6587\u7ae0\u63a8\u8350<\/span>\u3011<\/span><\/strong><\/p>\n

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

Jieyuan Li et al. Probing ring-opening pathways for efficient photocatalytic toluene decomposition, J. Mater. Chem. A, 2019,7, 3366-3374.<\/p>\n

\"\"<\/p>\n

Jieyuan Li et al. Cu supported on polymeric carbon nitride for selective CO2 <\/sub>reduction into CH4<\/sub>: a combined kinetics and thermodynamics investigation, J. Mater. Chem. A, 2019, 7, 17014.<\/p>\n

\"\"Jieyuan Li et al. The Spatially Oriented Charge Flow and Photocatalysis Mechanism on Internal van der Waals Heterostructures Enhanced g\u001eC3<\/sub>N4<\/sub>, ACS Catal., 2018, 8, 8376-8385.<\/p>\n

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

Jieyuan Li et al. Tailoring the rate-determining step in photocatalysis via localized excess electrons for efficient and safe air cleaning, Appl. Catal. B: Environ., 2018, 239, 187-195.<\/p>\n

\"\"<\/p>\n

Jieyuan\u00a0Li et al. Unraveling the Mechanism of Binary Channel Reactions in Photocatalytic Formaldehyde Decomposition for Promoted Mineralization, Appl. Catal. B: Environ., Accepted, DOI: 10.1016\/j.apcatb.2019.118130.<\/p>\n

\u672c\u6587\u7531\u56db\u5ddd\u5927\u5b66\u5efa\u7b51\u4e0e\u73af\u5883\u5b66\u9662<\/strong>\u4f9b\u7a3f\u3002<\/p>\n

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\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

\u6295\u7a3f\u4ee5\u53ca\u5185\u5bb9\u5408\u4f5c\u53ef\u52a0\u7f16\u8f91\u5fae\u4fe1\uff1acailiaorenVIP.<\/p>\n<\/section>\n","protected":false},"excerpt":{"rendered":"

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