{"id":98111,"date":"2017-08-28T06:30:49","date_gmt":"2017-08-27T22:30:49","guid":{"rendered":"\/\/m.iemloyee.com\/?p=98111"},"modified":"2017-08-24T13:07:41","modified_gmt":"2017-08-24T05:07:41","slug":"%e5%a4%a7%e8%bf%9e%e5%8c%96%e7%89%a9%e6%89%80%e6%9d%8e%e7%81%bf%e9%99%a2%e5%a3%abjacs%ef%bc%9a%e7%ad%89%e7%a6%bb%e5%ad%90%e6%bf%80%e5%85%83%e5%85%89%e5%82%ac%e5%8c%96%e4%b8%ad%e6%b0%b4%e6%b0%a7","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=98111","title":{"rendered":"\u5927\u8fde\u5316\u7269\u6240\u674e\u707f\u9662\u58ebJACS\uff1a\u7b49\u79bb\u5b50\u6fc0\u5143\u5149\u50ac\u5316\u4e2d\u6c34\u6c27\u5316\u53cd\u5e94\u6d3b\u6027\u4f4d\u70b9\u5b9a\u4f4d"},"content":{"rendered":"

\u4e03\u5915\u4f73\u8282\uff0c\u613f\u5929\u4e0b\u771f\u5fc3\u4eba\u90fd\u80fd\u6536\u83b7\u7f8e\u6ee1\u7684\u7231\u60c5\uff0c\u751c\u871c\u5e78\u798f\u957f\u957f\u4e45\u4e45\uff01\u6750\u6599\u4eba\u65f6\u523b\u4f34\u60a8\u5de6\u53f3\uff01<\/strong><\/span><\/p>\n

\u2014\u2014\u6750\u6599\u4eba\u7f16\u8f91\u90e8 \u00a0<\/span><\/p>\n

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

\u5728\u8868\u9762\u7b49\u79bb\u5b50\u5171\u632f\uff08SPR\uff09\u589e\u5f3a\u8fc7\u7a0b\u4e2d\uff0c\u7b49\u79bb\u5b50\u8bf1\u5bfc\u70ed\u7535\u8377\u5206\u79bb\uff08PICS\uff09\u673a\u5236\u88ab\u5e7f\u6cdb\u7814\u7a76\uff0c\u8fd9\u4e3b\u8981\u5f52\u56e0\u4e8ePICS\u80fd\u591f\u62d3\u5c55\u5149\u50ac\u5316\u5242\u7684\u5438\u6536\u5149\u8c31\uff0c\u901a\u8fc7\u6709\u6548\u63a7\u5236\u91d1\u5c5e\u7c92\u5b50\u7684\u5c3a\u5bf8\u548c\u5f62\u72b6\uff0c\u53ef\u4ee5\u8c03\u8282\u8fd9\u79cd\u62d3\u5c55\u7684\u53ef\u80fd\u6027\u3002\u5728PICS\u4e2d\uff0c\u7b49\u79bb\u5b50\u5171\u632f\u901a\u8fc7Landau\u963b\u5c3c\u6a21\u5f0f\u4ee5\u975e\u8f90\u5c04\u5f62\u5f0f\u5c06\u80fd\u91cf\u4f20\u9012\u7ed9\u4f4d\u4e8e\u91d1\u5c5e\u4e2d\u7684\u70ed\u7535\u5b50-\u7a7a\u7a74\u5bf9\uff0c\u8be5\u8fc7\u7a0b\u8017\u65f6\u6781\u77ed\uff0c\u53ef\u57281~100\u98de\u79d2\u5185\u5b8c\u6210\u3002\u70ed\u7535\u8377\u5982\u6b64\u77ed\u6682\u7684\u5bff\u547d\u4e25\u91cd\u5236\u7ea6\u4e86\u7b49\u79bb\u5b50\u5149\u50ac\u5316\u5242\u7684\u5e94\u7528\u3002\u901a\u8fc7\u5728\u7b49\u79bb\u5b50\u91d1\u5c5e\u7eb3\u7c73\u7c92\u5b50\u548c\u9002\u5f53\u7684\u534a\u5bfc\u4f53\u8f7d\u4f53\uff08\u5982\uff0cTiO2<\/sub>\uff09\u95f4\u6784\u5efa\u8096\u7279\u57fa\u63a5\u89e6\uff0c\u53ef\u4ee5\u5b9e\u73b0\u70ed\u7535\u5b50-\u7a7a\u7a74\u5bf9\u7684\u6709\u6548\u5206\u79bb\u3002\u8fd1\u51e0\u5e74\uff0c\u7814\u7a76\u4eba\u5458\u5bf9\u4e8eSPR\u7684\u70ed\u7535\u5b50\u8f6c\u79fb\u7684\u673a\u7406\u8ba4\u8bc6\u4e0d\u65ad\u63d0\u9ad8\uff0c\u5229\u7528\u70ed\u7535\u5b50\u9a71\u52a8\u6216\u589e\u5f3a\u50ac\u5316\u53cd\u5e94\u7684\u5e94\u7528\u4e5f\u5c61\u89c1\u62a5\u9053\u3002\u4f46\u662f\uff0c\u8981\u4f7f\u5f97SPR\u4ea7\u751f\u7684\u8f7d\u6d41\u5b50\u80fd\u8fdb\u884c\u9ad8\u6548\u7684\u5149\u50ac\u5316\u6c34\u5206\u89e3\u53cd\u5e94\uff0c\u5fc5\u987b\u7efc\u5408\u8ba4\u8bc6\u70ed\u7535\u5b50\u548c\u70ed\u7a7a\u7a74\u9a71\u52a8\u7684\u8868\u9762\u53cd\u5e94\u7684\u7269\u7406\u673a\u5236\u3002\u7a7a\u7a74\u9a71\u52a8\u7684\u6c34\u6c27\u5316\u53cd\u5e94\u4f5c\u4e3a\u592a\u9633\u80fd\u8f6c\u5316\u8fc7\u7a0b\u4e2d\u7684\u5173\u952e\u53cd\u5e94\uff0c\u4e86\u89e3\u5176\u80cc\u540e\u7684\u7269\u7406\u5316\u5b66\u673a\u5236\u663e\u5f97\u5c24\u4e3a\u91cd\u8981\u3002\u7136\u800c\u5230\u76ee\u524d\u4e3a\u6b62\uff0c\u5bf9\u4e8e\u70ed\u7a7a\u7a74\u7684\u8ba4\u8bc6\u8fd8\u5f88\u7f3a\u4e4f\uff0c\u7279\u522b\u662f\u5173\u4e8e\u70ed\u7a7a\u7a74\u7684\u5206\u5e03\u72b6\u6001\u4ee5\u53ca\u5176\u9a71\u52a8\u7684\u6c34\u6c27\u5316\u53cd\u5e94\u7684\u6d3b\u6027\u4f4d\u70b9\u7684\u8ba4\u8bc6\u4ecd\u4e0d\u6e05\u695a\u3002<\/p>\n

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

\u8fd1\u65e5\uff0c\u4e2d\u79d1\u9662\u5927\u8fde\u5316\u7269\u6240\u674e\u707f\u9662\u58eb\uff08\u901a\u8baf\u4f5c\u8005\uff09\u56e2\u961f<\/strong>\u5728J. Am. Chem. Soc.<\/em><\/strong>\u4e0a\u53d1\u8868\u4e86\u4e00\u7bc7\u9898\u4e3a\u201cPositioning the Water Oxidation Reaction Sites in Plasmonic Photocatalysts<\/strong>\u201d\u7684\u6587\u7ae0\u3002\u5728\u8be5\u6587\u4e2d\uff0c\u7814\u7a76\u4eba\u5458\u4ee5Au\/TiO2\u4e3a\u7b49\u79bb\u5b50\u5149\u50ac\u5316\u5242\u7684\u6807\u51c6\u6a21\u578b\uff0c\u5728\u5176\u8868\u9762\u8fdb\u884c\u9009\u62e9\u6027\u5149\u6c89\u79ef\uff0c\u7ed3\u5408HAADF-STEM\u53caEDS\u8868\u5f81\uff0c\u5b9e\u73b0\u4e86\u53cd\u5e94\u4f4d\u70b9\u7684\u5b9a\u4f4d\u3002\u6b64\u5916\uff0c\u7b49\u79bb\u5b50\u6240\u4ea7\u751f\u7684\u70ed\u7535\u5b50-\u7a7a\u7a74\u5bf9\u7684\u5206\u79bb\u548c\u5206\u5e03\u4e5f\u53ef\u4ee5\u5229\u7528KPFM\u76f4\u63a5\u6210\u50cf\u663e\u793a\u3002\u7814\u7a76\u4eba\u5458\u8bc1\u660e\u70ed\u7a7a\u7a74\u4e3b\u8981\u79ef\u805a\u5728\u8fd1\u754c\u9762\u533a\u57df\uff0c\u540c\u65f6\u6c34\u6c27\u5316\u53cd\u5e94\u6d3b\u6027\u4f4d\u70b9\u4e5f\u4f4d\u4e8eAu\/\u534a\u5bfc\u4f53\u754c\u9762\u5904\u3002\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u6a21\u62df\u8ba1\u7b97\u8fdb\u4e00\u6b65\u8bc1\u5b9e\u4e86\u7b49\u79bb\u5b50\u91d1\u5c5e\/\u534a\u5bfc\u4f53\u754c\u9762\u5728\u6c34\u6c27\u5316\u53cd\u5e94\u4e2d\u6240\u8d77\u7684\u4fc3\u8fdb\u4f5c\u7528\u3002<\/p>\n

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

\u56fe\u4e00<\/strong>\u00a0 <\/strong>\u7b49\u79bb\u5b50<\/strong>Au\/TiO2<\/strong>\u5149\u50ac\u5316\u5242\u7684\u6c34\u6c27\u5316\u6d3b\u6027\u6d4b\u8bd5<\/strong><\/p>\n

\"\"<\/p>\n

(A) <\/strong>\u5728\u53ef\u89c1\u5149\u7167\u5c04\uff08> 440nm\uff09\u4e0b\uff0cAu\/TiO2<\/sub>\u3001Au\/SiO2<\/sub>\u548cTiO2<\/sub>\u7684\u6c34\u6c27\u5316\u6bd4\u8f83\uff1b<\/p>\n

(B) <\/strong>\u5728\u7b49\u79bb\u5b50\u6fc0\u5143\u9a71\u52a8\u7684\u6c34\u6c27\u5316\u4e2d\uff0cAu\/TiO2<\/sub>\u7684\u5438\u6536\u5149\u8c31\uff08\u53f3\u8f74\uff09\u548c\u6d3b\u6027\u5149\u8c31\uff08\u5de6\u8f74\uff09\uff1b<\/p>\n

(C) <\/strong>\u91d1\u7ea2\u77f3\u76f8\u548c\u9510\u949b\u77ff\u76f8Au\/TiO2<\/sub>\u7684\u7b49\u79bb\u5b50\u57fa\u5143\u9a71\u52a8\u7684\u6c34\u6c27\u5316\u6d3b\u6027\u5bf9\u6bd4\uff1b<\/p>\n

(D) <\/strong>\u7d2b\u5916\u5149\u7167\uff08<400 nm\uff09\u4e0b\uff0c\u91d1\u7ea2\u77f3\u76f8\u548c\u9510\u949b\u77ff\u76f8TiO2<\/sub>\u7684\u6c34\u6c27\u5316\u6d3b\u6027\u5bf9\u6bd4\u3002<\/p>\n

\u56fe\u4e8c<\/strong>\u00a0 <\/strong>\u4e0d\u540c\u5149\u6c89\u79ef\u6761\u4ef6\u4e0b\u7684<\/strong>HAADF-STEM<\/strong>\u8868\u5f81\u53ca\u6c34\u6c27\u5316\u6027\u80fd\u7814\u7a76<\/strong><\/p>\n

\"\"<\/p>\n

(A-D) <\/strong>\u5229\u7528UV\uff08<400nm\uff09\u548c\u53ef\u89c1\u5149\uff08> 440nm\uff09\u5149\u6c89\u79ef\u540e\uff0cAu\/\u91d1\u7ea2\u77f3TiO2\u7684HAADF-STEM\u548cEDS\u5143\u7d20\u5206\u5e03\u8868\u5f81\u56fe\u50cf\uff1a<\/p>\n

\u00a0 \u00a0 \u00a0A\uff09Cr-UV\uff1a\u7d2b\u5916\u5149\u7167\u5c04\u4e0b\uff0cCr2<\/sub>O3<\/sub>\u5728Au\/TiO2<\/sub>\u4e0a\u7684\u5149\u8fd8\u539f\u6c89\u79ef\uff1b \u00a0 \u00a0 \u00a0 \u00a0\u00a0B\uff09Pb-vis\uff1a\u53ef\u89c1\u5149\u7167\u5c04\u4e0b\uff0cPbO2\u5728Au\/TiO2<\/sub>\u4e0a\u7684\u5149\u6c27\u5316\u6c89\u79ef\uff1b<\/p>\n

\u00a0 \u00a0 \u00a0C\uff09Cr-UV-200\uff1a200\u2103\u4e0b\uff0cCr-UV\u6837\u54c1\u5728\u7a7a\u6c14\u4e2d\u7145\u70e71 h\uff1b \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0 \u00a0\u00a0D\uff09Pb-vis-200\uff1a200\u2103\u4e0b\uff0cPb-vis\u6837\u54c1\u5728\u7a7a\u6c14\u4e2d\u7145\u70e71 h\uff1b<\/p>\n

(E) <\/strong>\u4e0d\u540c\u6761\u4ef6\u5904\u7406\u540e\u7684\u5149\u50ac\u5316\u5242\uff08A-D\uff09\u7684\u7b49\u79bb\u5b50\u6c34\u6c27\u5316\u6027\u80fd\uff0c<\/p>\n

\u56fe\u4e09<\/strong>\u00a0 Au\/TiO2<\/sub><\/strong>\u7684<\/strong>AFM<\/strong>\u3001<\/strong>KPFM<\/strong>\u53ca<\/strong>SPV<\/strong>\u8868\u5f81<\/strong><\/p>\n

\"\"<\/p>\n

(A) <\/strong>Au NP\u6c89\u79ef\u5728\u91d1\u7ea2\u77f3\u76f8TiO2<\/sub>\u5355\u6676\u4e0a\u7684AFM\u5f62\u8c8c\u56fe\uff0c\u5355\u4e2aAu NP\u7684\u9ad8\u5ea6\u5927\u7ea6\u4e3a68 nm\uff1b<\/p>\n

(B-C) <\/strong>\u4e0d\u540c\u5149\u7167\u4e0b\uff0cAu\/TiO2<\/sub>\u7684KPFM\u56fe\u50cf\uff1a\u9ed1\u6697\uff08B\uff09\uff1b532 nm \u5149\u7167\uff1b<\/p>\n

(D) <\/strong>\u4ece532 nm \u5149\u7167\u7535\u4f4d\u4e2d\u51cf\u53bb\u6697\u7535\u4f4d\u540e\uff0cAu\/TiO2<\/sub>\u7684SPV\u56fe\u50cf(SPV, \u0394CPD = CPDlight<\/sub>\u2013CPDdark<\/sub>)\uff1b<\/p>\n

(E) <\/strong>Au\/TiO2<\/sub> NP\u7684\u6697\u6001\uff08\u9ed1\u7ebf\uff09\u548c\u5149\u7167\u72b6\u6001\uff08\u7ea2\u7ebf\uff09\u7684\u63a5\u89e6\u7535\u4f4d\u5dee\uff08CPD\uff09\u66f2\u7ebf\u3002<\/p>\n

(F) <\/strong>\u4ece532 nm \u5149\u7167\u7535\u4f4d\u4e2d\u51cf\u53bb\u6697\u7535\u4f4d\u540e\uff0cAu\/TiO2<\/sub> NP\u7684SPV\u66f2\u7ebf\uff0c\u56fe\u4e2d\u7c89\u7ea2\u8272\u6807\u8bc6\u533a\u4ee3\u8868Au\/TiO2<\/sub>\u754c\u9762\u533a\u57df\u3002<\/p>\n

\u56fe\u56db<\/strong>\u00a0 Au\/TiO2<\/sub> <\/strong>\u5149\u50ac\u5316\u5242\u7684<\/strong>DFT<\/strong>\u8ba1\u7b97\u6a21\u62df\u7ed3\u679c<\/strong><\/p>\n

\"\"<\/p>\n

(A) <\/strong>Au8\u56e2\u7c07\u6c89\u79ef\u5728\u91d1\u7ea2\u77f3\u76f8TiO2<\/sub>\uff08110\uff09\u8868\u9762\u7684\u4f18\u5316\u7ed3\u6784\uff1b<\/p>\n

(B) <\/strong>Au8\/TiO2<\/sub>\u76f8\u5e94\u7684\u80fd\u5e26\u7ed3\u6784\uff1b<\/p>\n

(C) <\/strong>\u56fe\uff08B\uff09\u4e2d\u80fd\u5e26\u7ed3\u6784\u7684\u533a\u57df\u653e\u5927\u56fe\uff0c\u5728\u56fe\uff08B\uff09\u548c\uff08C\uff09\u4e2d\u7684\u8d39\u7c73\u80fd\u7ea7\u8bbe\u5b9a\u4e3a0 eV\uff1b<\/p>\n

(D) <\/strong>\u4e0e\u6c34\u6c27\u5316\u7535\u4f4d\uff081.23 eV, vs. RHE at pH 0\uff09\u76f8\u6bd4\uff0c<\/strong>Au8\/TiO2<\/sub>\u7684\u80fd\u5e26\u548cAu8\u5728TiO2<\/sub>\u4e0a\u5f62\u6210\u7684\u65b0\u6742\u5316\u6001\uff1b<\/p>\n

(E) <\/strong>Au\/TiO2<\/sub>\u8868\u9762\u4e0a\u6c34\u6c27\u5316\u673a\u5236\u7684\u81ea\u7531\u80fd\u56fe\u793a\u3002<\/p>\n

\u56fe\u4e94<\/strong>\u00a0 <\/strong>\u5176\u4ed6\u91d1\u8d1f\u8f7d\u6750\u6599\u7684\u7b49\u79bb\u5b50\u6c34\u6c27\u5316\u6d3b\u6027\u6d4b\u8bd5<\/strong><\/p>\n

\"\"<\/p>\n

(A) <\/strong>\u5728\u53ef\u89c1\uff08> 440 nm\uff09\u5149\u7167\u4e0b\uff0c\u5176\u4ed6\u91d1\u8d1f\u8f7d\u6750\u6599\u7684\u7b49\u79bb\u5b50\u6c34\u6c27\u5316\u6d3b\u6027\uff1b<\/p>\n

(B) <\/strong>\u5728\u53ef\u89c1\u5149\u7167\u5c04\u4e0b\uff0c\u5229\u7528\u6c27\u5316\u8fd8\u539f\u7535\u5bf9\u6eb6\u6db2\uff08Fe2+<\/sup>\/3+<\/sup>\uff09\uff0c Au\/TiO2\u4e0eSrTiO3\uff1aRh\u8026\u5408\u7684Z-scheme\u7ed3\u6784\u5149\u50ac\u5316\u5168\u5206\u89e3\u6c34\u4ea7\u751fH2<\/sub>\u548cO2<\/sub>\u7684\u5faa\u73af\u6d4b\u91cf\u3002<\/p>\n

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

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\u6587\u732e\u94fe\u63a5\uff1a<\/strong>Positioning the Water Oxidation Reaction Sites in Plasmonic Photocatalysts<\/a>(J. Am. Chem. Soc.<\/em>, 2017, DOI: 10.1021\/jacs.7b04470)<\/p>\n

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