{"id":249148,"date":"2023-03-30T06:16:59","date_gmt":"2023-03-29T22:16:59","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=249148"},"modified":"2023-03-28T15:17:21","modified_gmt":"2023-03-28T07:17:21","slug":"%e6%97%a5%e6%9c%ac%e5%8c%97%e6%b5%b7%e9%81%93%e5%a4%a7%e5%ad%a6acs-catal-%ef%bc%9afe-%e6%b2%b8%e7%9f%b3%e4%b8%8anh3-scr%e6%9c%ba%e7%90%86%e7%9a%84%e5%8e%9f%e4%bd%8d%e5%85%89%e8%b0%b1%e7%a0%94%e7%a9%b6","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=249148","title":{"rendered":"\u65e5\u672c\u5317\u6d77\u9053\u5927\u5b66ACS Catal.\uff1aFe-\u6cb8\u77f3\u4e0aNH3-SCR\u673a\u7406\u7684\u539f\u4f4d\u5149\u8c31\u7814\u7a76"},"content":{"rendered":"

\u4e00\u3001<\/b><\/strong>\u3010\u5bfc\u8bfb\u3011<\/b><\/strong><\/p>\n

\u5bcc\u6c27\u6761\u4ef6\u4e0b\uff0c\u5229\u7528\u6c28\u901a\u8fc7\u94c1\u6216\u94dc\u4ea4\u6362\u6cb8\u77f3\u9009\u62e9\u6027\u50ac\u5316\u8fd8\u539f\uff08NH3<\/sub>-SCR\uff09\u6c2e\u6c27\u5316\u7269\uff08NOx<\/sub>\uff09\uff0c\u5bf9\u4e8e\u63a7\u5236\u67f4\u6cb9\u8f66\u7684NOx<\/sub>\u6392\u653e\u81f3\u5173\u91cd\u8981\uff0c\u800c\u4f20\u7edf\u7684V2<\/sub>O5<\/sub>\u57fa\u50ac\u5316\u5242\u901a\u5e38\u4f5c\u4e3a\u56fa\u5b9a\u8131\u786b\u7cfb\u7edf\u4e2d\u7684\u5de5\u4e1a\u50ac\u5316\u5242\u3002\u5176\u4e2d\uff0c\u52a8\u529b\u5b66\u3001\u5149\u8c31\u548c\u7406\u8bba\u7814\u7a76\u5df2\u7ecf\u81f4\u529b\u4e8e\u5728\u5206\u5b50\u6c34\u5e73\u4e0a\u7406\u89e3NH3<\/sub>-SCR\u673a\u5236\uff08V2<\/sub>O5<\/sub>\uff0cCu\u548cFe\uff09\uff0c\u4ece\u800c\u5408\u7406\u8bbe\u8ba1NH3<\/sub>-SCR\u50ac\u5316\u5242\u3002\u5728\u4e4b\u524d\u7684\u7814\u7a76\u4e2d\u5df2\u7ecf\u5bf9\u4e09\u79cdSCR\u50ac\u5316\u5242\u7684\u673a\u7406\u8fdb\u884c\u4e86\u5145\u5206\u7684\u8ba8\u8bba\uff0c\u8fd9\u4e9b\u50ac\u5316\u5242\u7684NH3<\/sub>-SCR\u53ef\u80fd\u5b58\u5728\u5171\u540c\u7684\u673a\u7406\u3002\u57fa\u4e8e\u539f\u4f4d\u548c\u64cd\u4f5c\u5149\u8c31\u4ee5\u53ca\u7ed3\u5408\u5148\u524d\u7684\u7814\u7a76\uff0c\u8868\u660e\u50ac\u5316\u8fc7\u7a0b\u662f\u57fa\u4e8e\u91d1\u5c5e\u9633\u79bb\u5b50\u7684\u6c27\u5316\u8fd8\u539f\u8026\u5408\u8fc7\u7a0b\u3002\u540c\u65f6\uff0c\u5728Cu-\u6cb8\u77f3\u4e2d\uff0c\u4e00\u4e2aOH–<\/sup>\u914d\u4f4d\u7684Cu2+<\/sup>\u9633\u79bb\u5b50\uff08Cu2+<\/sup>(OH–<\/sup>)\uff09\u88ab\u786e\u5b9a\u4e3a\u8fd8\u539f\u534a\u5faa\u73af\uff08RHC\uff09\u7684\u6d3b\u6027\u4f4d\u70b9\u3002\u4e0e\u8bb8\u591a\u4f7f\u7528\u539f\u4f4d\u5149\u8c31\u548c\u7406\u8bba\u65b9\u6cd5\u62a5\u9053\u7684\u94dc\u57fa\u50ac\u5316\u5242\u76f8\u6bd4\uff0c\u5f88\u5c11\u6709\u5b9e\u9a8c\u548c\u7406\u8bba\u7814\u7a76\u96c6\u4e2d\u5728\u57fa\u4e8eFe-\u6cb8\u77f3\u7684NH3<\/sub>-SCR\u4e2d\u7684RHC\u3002<\/p>\n

\u4e8c\u3001<\/b><\/strong>\u3010\u6210\u679c\u63a0\u5f71\u3011<\/b><\/strong><\/p>\n

\u5728\u6b64\uff0c\u65e5\u672c\u5317\u6d77\u9053\u5927\u5b66Ken-ichi Shimizu\u6559\u6388<\/strong>\u91c7\u7528\u539f\u4f4d\/\u64cd\u4f5c\u5149\u8c31\uff08\u7ea2\u5916\u3001\u7d2b\u5916\u548cFe-edge X\u5c04\u7ebf\u5438\u6536\u8fd1\u8fb9\u7ed3\u6784\uff09\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\uff0c\u7814\u7a76\u4e86\u5728300\u2103\u4e0bNH3<\/sub>\uff08NH3<\/sub>-SCR\uff09\u5bf9\u94c1\u4ea4\u6362\u4e1d\u5149\u6cb8\u77f3\uff08MOR\uff09\u5206\u5b50\u7b5b\u9009\u62e9\u6027\u50ac\u5316\u8fd8\u539fNO\u7684\u8fd8\u539f\/\u6c27\u5316\u534a\u5faa\u73af\u3002\u4e0d\u540c\u7684\u5149\u8c31\u7ed3\u679c\u8868\u660e\uff0c\u5728\u8fd8\u539f\u534a\u5faa\u73af\uff08NO+NH3<\/sub>\uff09\u4e2d\uff0cFe3+<\/sup>\u8fd8\u539f\u4e3aFe2+<\/sup>\uff0c\u540c\u65f6\u5f62\u6210N2<\/sub>\u548cH2<\/sub>O\u3002\u5728\u968f\u540e\u7684\u6c27\u5316\u534a\u5faa\u73af\u4e2d\uff08\u5728O2<\/sub>\u6216NO+O2<\/sub>\u4e0b\uff09\uff0cFe2+<\/sup>\u88ab\u518d\u6c27\u5316\u4e3aFe3+<\/sup>\u3002\u8fd8\u539f\u534a\u5faa\u73af\u5305\u62ec\u51e0\u4e2a\u57fa\u672c\u6b65\u9aa4\u3002\u5728\u4f4e\u6e29\uff08<100\u2103\uff09\u4e0b\uff0cFe3+<\/sup>-OH\u8fd8\u539f\u4ea7\u751fFe2+<\/sup>\u548cNO+<\/sup>\uff0c\u800c\u5728100\u2103\u7684NH3<\/sub>\u66b4\u9732\u4e0b\uff0c\u89c2\u5bdf\u5230NO+<\/sup>\u8fd8\u539f\u9a71\u52a8N2<\/sub>\u5f62\u6210\u3002\u5728\u77ac\u6001\u6761\u4ef6\u4e0b\uff0c\u5f53B-NH3<\/sub>\u8986\u76d6\u7387\u8f83\u4f4e\u65f6\uff0cBr\u00f8nsted\u9178\u4f4d\u70b9\uff08B-NH3<\/sub>\uff09\u4e0a\u7684\u6c28\u4e0eNO\u53cd\u5e94\u751f\u6210N2<\/sub>\uff0c\u8868\u660eB-NH3<\/sub>\u4f1a\u53c2\u4e0e\u53cd\u5e94\u3002\u540c\u65f6\uff0c\u8fc7\u6e21\u6001\u8ba1\u7b97\u7406\u8bba\u4e0a\u8868\u660e\uff0c\u7531[Fe3+<\/sup>(OH–<\/sup>)2<\/sub>]+<\/sup>\u548c\u6c14\u6001NO\u5f62\u6210\u4e9a\u785d\u9178\uff08HONO\uff09\u4e2d\u95f4\u4f53\u662f\u4e00\u4e2a\u7b80\u5355\u7684\u8fc7\u7a0b\uff08Ea<\/sub>=29.2 kJ\/mol\uff09\u3002\u7ed3\u5408\u5b9e\u9a8c\u89c2\u5bdf\u548cDFT\u8ba1\u7b97\uff0c\u672c\u6587\u63d0\u51fa\u4e86Fe-\u6cb8\u77f3\u4e0a\u8fd8\u539f\u534a\u5faa\u73af\u7684\u673a\u7406\uff1a[Fe<\/strong>3+<\/sup><\/strong>(OH<\/strong>–<\/sup><\/strong>)<\/strong>2<\/sub><\/strong>]<\/strong>+<\/sup><\/strong>\u88abNO\u8fd8\u539f\u751f\u6210HONO\u4e2d\u95f4\u4f53\uff0cHONO\u4e2d\u95f4\u4f53\u4e0eBr\u00f8nsted\u9178\u4f4d\u70b9\u4e0a\u7684NH<\/strong>3<\/sub><\/strong>\u53cd\u5e94\uff0c\u901a\u8fc7NO<\/strong>+<\/sup><\/strong>\u751f\u6210H<\/strong>2<\/sub><\/strong>O\u548cN<\/strong>2<\/sub><\/strong>\u3002\u57fa\u4e8e\u4e0a\u8ff0\u673a\u7406\u89c1\u89e3\uff0c\u5bf9\u4e0d\u540cFe\u8377\u8f7d\u548cSi\/Al\u6bd4\u7684Fe-\u6cb8\u77f3\uff08MOR\u548c\u03b2\uff09\u8fdb\u884c\u4e86NH3<\/sub>-SCR\u53cd\u5e94\u3002\u7ed3\u679c\u8868\u660e\uff0c\u5177\u6709\u5927\u91cfBr\u00f8nsted\u9178\u4f4d\u70b9\u7684\u542b2.7 wt %\u94c1-\u6cb8\u77f3\uff08Si\/Al\u6bd4\u4e3a5\uff09\uff0c\u5728\u4f4e\u6e29\u533a\u57df\u663e\u793a\u51fa\u6700\u9ad8\u7684NOx<\/sub>\u8f6c\u5316\u7387\u3002<\/p>\n

\u76f8\u5173\u7814\u7a76\u6210\u679c\u4ee5\u201cIn Situ<\/i><\/em><\/strong>\/Operando Spectroscopic Studies on the NH<\/strong>3<\/sub><\/strong>–<\/strong>SCR Mechanism over Fe<\/strong>–<\/strong>Zeolites<\/strong>\u201d\u4e3a\u9898\u53d1\u8868\u5728ACS Catal.<\/i><\/em><\/strong>\u4e0a\u3002\"\"<\/p>\n

\u4e09\u3001<\/b><\/strong>\u3010\u6838\u5fc3\u521b\u65b0\u70b9\u3011<\/b><\/strong><\/p>\n

1.\u672c\u6587\u91c7\u7528\u539f\u4f4d\/\u64cd\u4f5c\u5149\u8c31\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\u8ba1\u7b97\u7ed3\u5408\u7684\u65b9\u5f0f\uff0c\u7814\u7a76\u4e86\u5728300\u2103\u4e0bNH3<\/sub>\u5bf9\u94c1\u4ea4\u6362\u4e1d\u5149\u6cb8\u77f3\uff08MOR\uff09\u5206\u5b50\u7b5b\u9009\u62e9\u6027\u50ac\u5316\u8fd8\u539fNO\u7684\u8fd8\u539f\/\u6c27\u5316\u534a\u5faa\u73af\u3002<\/p>\n

2.\u672c\u6587\u63d0\u51fa\u4e86Fe-\u6cb8\u77f3\u4e0a\u8fd8\u539f\u534a\u5faa\u73af\u7684\u673a\u7406\uff0c\u4e14\u80fd\u591f\u5728\u4f4e\u6e29\u533a\u57df\u663e\u793a\u51fa\u6700\u9ad8\u7684NOx<\/sub>\u8f6c\u5316\u7387\u3002<\/p>\n

\u56db\u3001<\/b><\/strong>\u3010\u6570\u636e\u6982\u89c8\u3011<\/b><\/strong>\"\"<\/p>\n

\u56fe<\/b><\/strong>1<\/b> \u5df2\u62a5\u9053\u7684NH3<\/sub>-SCR\u673a\u7406\u00a9 2022 American Chemical Society <\/b><\/strong><\/p>\n

\uff08a\uff09\u62a5\u9053\u4e86NH3<\/sub>-SCR\u901a\u8fc7Cu2+<\/sup>-NH3<\/sub>\u4e2d\u95f4\u4f53\u5bf9Cu-CHA\u7684\u4f5c\u7528\u673a\u5236\uff1b<\/p>\n

\uff08b\uff09\u62a5\u9053\u4e86NH3<\/sub>-SCR\u901a\u8fc7\u79fb\u52a8\u7684HONO\u4e2d\u95f4\u4f53\u5bf9Cu-CHA\u7684\u4f5c\u7528\u673a\u5236\uff1b<\/p>\n

\uff08c\uff09\u62a5\u9053\u4e86NH3<\/sub>-SCR\u79fb\u52a8\u7684HONO\u4e2d\u95f4\u4f53\u5bf9Fe-Zeolite\u7684\u4f5c\u7528\u673a\u5236\u3002\"\"<\/b><\/strong><\/p>\n

\u56fe<\/b><\/strong>2 \u76f8\u5e94\u7684\u7ea2\u5916\u5149\u8c31\u7814\u7a76\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\uff08a\uff09\u5728500\u2103\u4e0b\uff0cFe1.3MOR10\u548cHMOR10\u8fd8\u539f0.1% NO\u65f6\u7684NO2<\/sub>\u7684\u6f14\u5316\uff1b<\/p>\n

\uff08b\uff09\u5728500\u2103\u4e0b\uff0c\u5c06Fe1.3MOR10\u8fd8\u539f0.1% NO+0.1%NH3<\/sub>\u65f6\uff0c\u51fa\u53e3\u6c14\u4f53\u4e2dNO\u548cNH3<\/sub>\u7684\u6d53\u5ea6\u4ee5\u53caN2<\/sub>\u548cH2<\/sub>O\u7684MS\u5f3a\u5ea6\uff1b<\/p>\n

\uff08c\uff09\u572835\u2103\u548c0.1%NO\u6761\u4ef6\u4e0b\uff0c\u5438\u9644\u7269\u8d28\u5728Fe1.3MOR10\u4e0a\u7684\u7ea2\u5916\u5149\u8c31\u3002\"\"<\/p>\n

\u56fe<\/b><\/strong>3 <\/b><\/strong>Fe1.3MOR10\u5728500<\/b><\/strong>\u2103<\/b><\/strong>\u548c<\/b><\/strong>10% O<\/b><\/strong>2<\/b><\/sub><\/strong>\uff081 min\uff09\u548c0.1% NO\uff081 min\uff09\u6761\u4ef6\u4e0b\u7684\u539f\u4f4d<\/b><\/strong>Fe-edge <\/b><\/strong>XANES\u5149\u8c31<\/b><\/strong>\u00a9 2022 American Chemical Society<\/b><\/strong>\"\"<\/p>\n

\u56fe<\/b><\/strong>4 300<\/b><\/strong>\u2103<\/b><\/strong>\u4e0b\u539f\u4f4dFe K-edge XANES\u6d4b\u91cf\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\uff08a-c\uff09\u5728300\u2103\u4e0b\uff0c\u8fde\u7eed\u52a0\u51650.1% NO\uff08500s\uff09\u30010.1%NO+0.1%\u00a0NH3<\/sub>\uff08950 s\uff09\u3001He\uff08600 s\uff09\u548c10% O2<\/sub>\u65f6Fe1.3MOR10\u7684Fe\u00a0k-edge XANES\u56fe\u8c31\u7684\u6f14\u5316\uff1b<\/p>\n

\uff08d-e\uff09\u5206\u522b\u57280.1% NO\u30010.1%NO+0.1%\u00a0NH3<\/sub>\u548c10% O2<\/sub>\u4e2dXANES\u80fd\u91cf\u7684\u53d8\u5316\u3002\"\"<\/p>\n

\u56fe<\/b><\/strong>5 \u7d2b\u5916-\u53ef\u89c1\u5149\u8c31\u7684\u6f14\u5316\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\uff08a-c\uff09\u5728300\u2103\u4e0b\uff0c\u4e0d\u540cFe1.3MOR10\u7684\u7d2b\u5916-\u5149\u8c31\u7684\u6f14\u5316\uff1b<\/p>\n

\uff08d\uff09\u5728265 nm\u5904\u7d2b\u5916-\u5f3a\u5ea6\u7684\u53d8\u5316\u8fc7\u7a0b\uff1b<\/p>\n

\uff08e\uff09\u5728O2<\/sub>\u6216NO+O2<\/sub>\u4e0b265 nm\u7d2b\u5916-\u5f3a\u5ea6\u7684\u65f6\u95f4\u8fc7\u7a0b\uff1b<\/p>\n

\uff08f\uff09\u5728265 nm\u5904\u7684\u7d2b\u5916-\u76f8\u5bf9\u5f3a\u5ea6\u548cN2<\/sub>\u7684\u8d28\u8c31\u5f3a\u5ea6\u7684\u65f6\u95f4\u8fc7\u7a0b\"\"<\/p>\n

\u56fe<\/b><\/strong>6 \u7ea2\u5916\u5149\u8c31\u6d4b\u8bd5\u00a9 2022 American Chemical Society <\/b><\/strong><\/p>\n

\uff08a\uff0cc\uff09\u57280.1% NO\u548c100\u2103\u4e0b\uff0c\u5438\u9644\u4e86NOx<\/sub>\u548c\u5176\u4ed6\u7269\u8d28\u7684\u7ea2\u5916\u5149\u8c31\uff1b<\/p>\n

\uff08b\uff09NO+<\/sup>\u548cFe2+<\/sup>-NO\u7684\u7ea2\u5916\u5cf0\u9ad8\u5ea6\u3002\"\"<\/p>\n

\u56fe<\/b><\/strong>7 T5\u56e2\u7c07<\/b>\u6a21\u578b\u5b9e\u73b0\u8fc7\u6e21\u6001\u8ba1\u7b97\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\uff08a\uff09\u4f7f\u7528\u4e86T5\u805a\u7c7b\u6a21\u578b\u7684MOR\u6cb8\u77f3\u6846\u67b6\uff1b<\/p>\n

\uff08b\uff09\u7531HONO\u5f62\u6210\u7684\u80fd\u91cf\u56fe\u3002\"\"<\/p>\n

\u56fe<\/b><\/strong>8<\/b><\/strong> Fe1.3MOR10\u7684\u7ea2\u5916\u6d4b\u8bd5\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\uff08a\uff09Fe1.3MOR10\u5438\u9644\u7269\u8d28\u7684\u7ea2\u5916\u5149\u8c31\uff1b<\/p>\n

\uff08b\uff09\u968f\u65f6\u95f4\u53d8\u5316\u7684NO+<\/sup>\u7684\u7ea2\u5916\u5cf0\u503c\u9ad8\u5ea6\u3002\"\"<\/p>\n

\u56fe<\/b><\/strong>9 \u5728200<\/b><\/strong>\u2103<\/b><\/strong>\u6761\u4ef6\u4e0bNH<\/b><\/strong>3<\/b><\/sub><\/strong>\u5438\u9644Fe1.3MOR10\u7684\u539f\u4f4d\u7ea2\u5916\u5b9e\u9a8c\u00a9 2022 American Chemical Society<\/b><\/strong>\"\"<\/p>\n

\u56fe<\/b><\/strong>10 \u5728300<\/b><\/strong>\u2103<\/b><\/strong>\u4e0bFe1.3MOR10\u4e0a\u7684\u8fde\u7eedRHC\/OHC\u8fc7\u7a0b\u7684\u539f\u4f4d\u7ea2\u5916\u5b9e\u9a8c\u00a9 2022 American Chemical Society<\/b><\/strong>\"\"<\/p>\n

\u56fe<\/b><\/strong>11 NH<\/b><\/strong>3<\/b><\/sub><\/strong>-SCR\u7ecf40 mg\u50ac\u5316\u5242\u5904\u7406\u540eNO<\/b><\/strong>x<\/b><\/sub><\/strong>\u8f6c\u5316\u4e0e\u6e29\u5ea6\u7684\u5173\u7cfb<\/b><\/strong>\u00a9 2022 American Chemical Society<\/b><\/strong><\/p>\n

\u4e94\u3001<\/b><\/strong>\u3010\u6210\u679c\u542f\u793a\u3011<\/b><\/strong><\/p>\n

\u7efc\u4e0a\u6240\u8ff0\uff0c\u672c\u6587\u57fa\u4e8e\u539f\u4f4d\/\u64cd\u4f5c\u5149\u8c31\u7814\u7a76\u7684\u7ed3\u679c\uff0c\u63d0\u51fa\u4e86NH3<\/sub>-SCR\u5728Fe-\u6cb8\u77f3\u4e0a\u7684\u4f5c\u7528\u673a\u7406\u3002[Fe3+<\/sup>(OH–<\/sup>)2<\/sub>]+<\/sup>\u88abNO\u8fd8\u539f\u751f\u6210HONO\u4e2d\u95f4\u4f53\uff0cHONO\u4e2d\u95f4\u4f53\u4e0eBr\u00f8nsted\u9178\u4f4d\u70b9\u4e0a\u7684NH3<\/sub>\u53cd\u5e94\uff0c\u901a\u8fc7NO+<\/sup>\u751f\u6210H2<\/sub>O\u548cN2<\/sub>\u5728\u4e0a\u8ff0RHC\u4e4b\u540e\uff0c\u662f[Fe2+<\/sup>(OH–<\/sup>)]+<\/sup>\u88abO2<\/sub>\u6216NO+O2<\/sub>\u6c27\u5316\u3002\u5728\u77ac\u6001\u6761\u4ef6\u4e0b\uff0cBASs\u4e0a\u7684\u6c28\u4f5c\u4e3a\u6c28\u7684\u50a8\u6c60\uff0c\u4e0eNO\u53cd\u5e94\u751f\u6210N2<\/sub>\uff0c\u8fd9\u53ef\u80fd\u5f97\u76ca\u4e8e\u901a\u8fc7\u5438\u9644\u7684\u6c28\u4e0e\u53ef\u79fb\u52a8\u7684HONO\u4e2d\u95f4\u4f53\u7684\u53cd\u5e94\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1a\u201c<\/strong>In Situ<\/i><\/u><\/em><\/strong>\/Operando Spectroscopic Studies on the NH<\/u><\/strong>3<\/sub><\/u><\/strong>–<\/u><\/strong>SCR Mechanism over Fe<\/u><\/strong>–<\/u><\/strong>Zeolites<\/u><\/strong><\/a>\u201d<\/strong>\uff08<\/strong>ACS Catal.<\/i><\/em><\/strong>\uff0c<\/b><\/strong>202<\/strong>2<\/strong>\uff0c<\/strong>10.1021\/acscatal.2c02904<\/strong>\uff09<\/strong><\/p>\n

\u672c\u6587\u7531\u6750\u6599\u4ebaCYM\u7f16\u8bd1\u4f9b\u7a3f\u3002<\/p>\n

 <\/p>\n","protected":false},"excerpt":{"rendered":"

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