{"id":263251,"date":"2024-11-08T06:06:10","date_gmt":"2024-11-07T22:06:10","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=263251"},"modified":"2024-11-07T21:13:16","modified_gmt":"2024-11-07T13:13:16","slug":"%e9%a6%99%e6%b8%af%e5%9f%8e%e5%b8%82%e5%a4%a7%e5%ad%a6%e5%bd%ad%e5%92%8f%e5%ba%b7%e8%af%be%e9%a2%98%e7%bb%84acs-catalysis%ef%bc%9a%e4%bb%8e%e5%8e%9f%e5%ad%90%e8%a7%86%e8%a7%92%e6%8e%a2%e7%a9%b6","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=263251","title":{"rendered":"\u9999\u6e2f\u57ce\u5e02\u5927\u5b66\u5f6d\u548f\u5eb7\u8bfe\u9898\u7ec4ACS Catalysis\uff1a\u4ece\u539f\u5b50\u89c6\u89d2\u63a2\u7a76\u8148\u7c7b\u6c34\u89e3\u7684CeO2\u8868\u9762\u4f9d\u8d56\u6027\u5728\u78b3\u9178\u4e8c\u7532\u916f\u5408\u6210\u4e2d\u7684\u4f5c\u7528"},"content":{"rendered":"

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

\u78b3\u9178\u4e8c\u7532\u916f\uff08DMC\uff09\u4f5c\u4e3a\u4e00\u79cd\u91cd\u8981\u7684\u5316\u5de5\u539f\u6750\u6599\uff0c\u5728\u6eb6\u5242\u3001\u805a\u5408\u7269\u5408\u6210\u3001\u71c3\u6599\/\u7535\u6c60\u6dfb\u52a0\u5242\u7b49\u9886\u57df\u5177\u6709\u5e7f\u6cdb\u5e94\u7528\u3002\u7136\u800c\uff0c\u4f20\u7edf\u7684DMC\u751f\u4ea7\u65b9\u6cd5\u4f9d\u8d56\u4e8e\u4f7f\u7528\u5371\u9669\u548c\u6613\u7206\u7684\u5316\u5b66\u54c1\uff0c\u5982\u5149\u6c14\u548cCO\u3002\u4e3a\u4e86\u5e94\u5bf9\u8fd9\u4e9b\u95ee\u9898\uff0c\u76f4\u63a5\u5229\u7528\u7532\u9187\u548cCO2<\/sub>\u5408\u6210DMC\u7684\u65b9\u6cd5\u5907\u53d7\u5173\u6ce8\u3002\u4f46\u662f\uff0c\u53d7\u70ed\u529b\u5e73\u8861\u7684\u4e25\u91cd\u9650\u5236\uff0cDMC\u7684\u4ea7\u7387\u5f88\u4f4e\u3002\u4e3a\u4e86\u514b\u670d\u8fd9\u4e00\u96be\u70b9\uff0c\u901a\u5e38\u4f1a\u5728\u5408\u6210\u8fc7\u7a0b\u4e2d\u5f15\u5165\u8131\u6c34\u5242\uff0c\u5176\u4e2d2-Cp\u8868\u73b0\u51fa\u6700\u4f73\u7684\u8131\u6c34\u6548\u679c\uff0c\u5e76\u4e14\u53ef\u91cd\u590d\u4f7f\u7528\u3002\u6709\u8da3\u7684\u662f\uff0cCeO2<\/sub>\u4e0d\u4ec5\u53ef\u4ee5\u50ac\u5316DMC\u7684\u5408\u6210\uff0c\u8fd8\u80fd\u4fc3\u8fdb2-Cp\u7684\u6c34\u89e3\u53cd\u5e94\uff0c\u5176\u53cd\u5e94\u6d3b\u6027\u8d85\u8fc7\u4e00\u822c\u7684\u6c27\u5316\u7269\u50ac\u5316\u5242\u3002\u5bf9\u4e8eDMC\u7684\u5408\u6210\uff0c\u6211\u4eec\u56e2\u961f\u4e4b\u524d\u7684\u7814\u7a76\u8868\u660e\uff0c\u7532\u9187\u7684\u6d3b\u5316\u662f\u5173\u952e\u6b65\u9aa4 [Appl. <\/em>Catal., B <\/em>2023, 336<\/em>, No. 122914.]\u3002\u7136\u800c\uff0c\u7531\u4e8e\u4ee5\u5f80\u7684\u7814\u7a76\u9ad8\u5ea6\u4f9d\u8d56NH3<\/sub>\/CO2<\/sub>-\u7a0b\u5e8f\u5347\u6e29\u8131\u9644\uff0c2-Cp\u6c34\u89e3\u6d3b\u6027\u7684\u5173\u952e\u56e0\u7d20\u5c1a\u4e0d\u660e\u786e\u3002\u4e3a\u4e86\u89e3\u51b3\u8fd9\u4e00\u95ee\u9898\uff0c\u672c\u5de5\u4f5c\u901a\u8fc7\u8c03\u63a7CeO2<\/sub>\u66b4\u9732\u7684\u6676\u9762\uff0c\u83b7\u5f97\u4e0d\u540c\u914d\u4f4d\u7ed3\u6784\u7684Ce\u4f4d\u70b9\uff0c\u5e76\u7ed3\u5408\u7535\u5b50\u987a\u78c1\u5171\u632f\uff08EPR\uff09\u3001X\u5c04\u7ebf\u5149\u7535\u5b50\u80fd\u8c31\uff08XPS\uff09\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u7b49\u591a\u79cd\u8868\u5f81\u624b\u6bb5\uff0c\u63ed\u793a\u4e862-Cp\u5728CeO2<\/sub>\u8868\u9762\u7684\u534f\u540c\u5438\u9644\u5bf9\u4e8e\u6676\u683c\u6c27\u7684\u4eb2\u6838\u52a0\u6210\u8d77\u7740\u5173\u952e\u4f5c\u7528\u3002<\/p>\n

\"\"<\/p>\n

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

\u4f17\u6240\u5468\u77e5\uff0c\u5728\u591a\u76f8\u50ac\u5316\u4e2d\uff0c\u53cd\u5e94\u7269\u7684\u5438\u9644\u548c\u6d3b\u5316\u4e0e\u56fa\u4f53\u50ac\u5316\u5242\u8868\u9762\u6d3b\u6027\u4f4d\u70b9\u7684\u914d\u4f4d\u7ed3\u6784\u5bc6\u5207\u76f8\u5173\u3002\u672c\u7814\u7a76\u91c7\u7528\u5177\u6709\u4f18\u79c0\u5f62\u8c8c\u63a7\u5236\u7684\uff0c\u4ee5\uff08111\uff09\u3001\uff08110\uff09\u548c\uff08100\uff09\u4e3a\u4e3b\u8981\u8868\u9762\u7684CeO2<\/sub>\u7eb3\u7c73\u9897\u7c92\uff0c\u63a2\u7d22Ce\u914d\u4f4d\u7ed3\u6784\u4e0e2-Cp\u6c34\u89e3\u6d3b\u6027\u7684\u5173\u7cfb\u3002\u52a8\u529b\u5b66\u7814\u7a76\u8868\u660e\uff0c2-Cp\u6c34\u89e3\u7684\u901f\u7387\u5e38\u6570\uff08k\uff09\u4e0e\u50ac\u5316\u5242\u8868\u9762\u76f8\u5173\uff0c\u5176\u4e2d\uff08111\uff09\u9762\u8868\u73b0\u51fa\u6700\u9ad8\u7684\u50ac\u5316\u6d3b\u6027\uff0c\u5176\u6b21\u662f\uff08110\uff09\u9762\uff0c\u800c\uff08100\uff09\u9762\u5728\u5ba4\u6e29\u4e0b\u51e0\u4e4e\u6ca1\u6709\u6d3b\u6027\u3002\u6b64\u5916\uff0c\u4e09\u79cd\u8868\u9762\u5728\u6c27\u7a7a\u4f4d\u3001Ce3+<\/sup>\/Ce4+<\/sup>\u6bd4\u7387\u548c\u7f9f\u57fa\u7b49\u6574\u4f53\u6027\u8d28\u4e0a\u76f8\u4f3c\uff0c\u65e0\u6cd5\u89e3\u91ca\u5176\u6d3b\u6027\u5dee\u5f02\u3002\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\u663e\u793a\uff0c\u5728\uff08110\uff09\u548c\uff08111\uff09\u9762\uff0c\u6c30\u57fa-N\u4e0e\u5421\u5576-N\u7684\u534f\u540c\u5438\u9644\u662f\u540e\u7eed\u8fdb\u884c\u6676\u683c\u6c27\u4eb2\u6838\u52a0\u6210\u7684\u5173\u952e\u6784\u578b\u3002\u5c3d\u7ba1\u8fd9\u4e24\u4e2a\u8868\u9762\u6240\u9700\u7684Ea\u76f8\u8fd1\uff0c\u4f46\u7531\u4e8e\u72ec\u7279\u7684Ce\u914d\u4f4d\u7ed3\u6784\u548c\u8868\u9762\u6392\u5217\uff0c\uff08111\uff09\u9762\u8868\u73b0\u51fa\u66f4\u6709\u6548\u76842-Cp\u6d3b\u5316\u80fd\u529b\u3002\u540c\u65f6\uff0c\uff08110\uff09\u9762\u57282-\u5421\u5576\u7532\u9170\u80fa\uff082-PA\uff09\u8131\u9644\u9636\u6bb5\u9700\u8981\u66f4\u9ad8\u7684\u80fd\u91cf\uff0c\u8fd9\u4e24\u70b9\u5171\u540c\u89e3\u91ca\u4e86\u4e3a\u4ec0\u4e48\uff08111\uff09\u9762\u8868\u73b0\u51fa\u66f4\u9ad8\u7684\u6c34\u89e3\u6d3b\u6027\u3002\u800c\u5728\uff08100\uff09\u9762\u4e0a\uff0c \u7f3a\u5c112-Cp\u7684\u534f\u540c\u5438\u9644\uff0c\u4f7f\u5f972-Cp\u7684\u6c34\u89e3\u53ea\u80fd\u901a\u8fc7\u8def\u6613\u65af\u9178\uff08Lewis acid\uff09\u6d3b\u5316\u9014\u5f84\u5b8c\u6210\uff0c\u8fd9\u9700\u8981\u7684\u8f83\u9ad8Ea\uff0c\u56e0\u6b64\u5bfc\u81f4\u4e86\uff08100\uff09\u9762\u7684\u4f4e\u6d3b\u6027\u3002<\/p>\n

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

\u628a\u4e0d\u540c\u6676\u9762\u7684CeO2<\/sub>\u7528\u57282-\u6c30\u57fa\u5421\u5576\uff082-Cp\uff09\u6c34\u89e3\u7684\u53cd\u5e94\u4e2d\uff0c\u5e76\u7814\u7a76\u4e86\u50ac\u5316\u5242\u8868\u9762\u7684Ce\u914d\u4f4d\u7ed3\u6784\u5bf9\u8be5\u53cd\u5e94\u7684\u5f71\u54cd\u3002<\/p>\n

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

\u5728\u4e0d\u540c\u7684CeO2<\/sub>\u6676\u9762\u4e0a\uff0cCe\u4f4d\u70b9\u5c55\u73b0\u51fa\u4e0d\u540c\u7684\u914d\u4f4d\u7ed3\u6784\uff0c\u5373\u5176\u7a7a\u8f68\u9053\u7684\u7a7a\u95f4\u7ed3\u6784\u548c\u6570\u76ee\u5b58\u5728\u5dee\u5f02\u3002\u5728\uff08111\uff09\u9762\u4e0a\uff0c\u4e00\u4e2aCe\u4f4d\u70b9\u4ec5\u6709\u4e00\u4e2a\u5782\u76f4\u4e8e\u8868\u9762\u7684\u7a7a\u8f68\u9053\uff1b\u800c\u5728\uff08110\uff09\u548c\uff08100\uff09\u9762\u4e0a\uff0c\u4e00\u4e2aCe\u4f4d\u70b9\u5219\u5177\u67092\u4e2a\u7a7a\u8f68\u9053\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\uff08110\uff09\u548c\uff08100\uff09\u9762\u7684\u7a7a\u8f68\u9053\u7684\u7a7a\u95f4\u7ed3\u6784\u662f\u4e0d\u540c\u7684\u3002\u5728\uff08110\uff09\u9762\u4e0a\uff0c\u4e00\u4e2aCe\u4f4d\u70b9\u62e5\u67092\u4e2a\u503e\u659c\u7684\u7a7a\u8f68\u9053\uff0c\u800c\u5728\uff08100\uff09\u9762\u4e0a\uff0c\u4e00\u4e2a\u6c27\u7a7a\u4f4d\u8fde\u63a5\u4e862\u4e2aCe\u4f4d\u70b9\u3002<\/p>\n

\"\"<\/p>\n

Scheme 1.<\/strong> Illustration of Ce coordination structures (with highlighted local geometry of vacant orbitals) and their arrangements on CeO2<\/sub> (a) (111), (b) (110), and (c) (100) surfaces.<\/p>\n

\u672c\u6587\u5408\u6210\u4e86\u4e09\u79cd\u5f62\u8c8c\u7684CeO2<\/sub>\uff0c\u8fd9\u4e9bCeO2<\/sub>\u66b4\u9732\u4e86\u4e0d\u540c\u7684\u6676\u9762\uff0c\u5373\uff08111\uff09\u3001\uff08110\uff09\u3001\uff08100\uff09\u9762\u3002\u8fd9\u4e09\u79cd\u6676\u9762\u7684CeO2<\/sub>\u57282-Cp\u6c34\u89e3\u4e2d\u7684\u6d3b\u6027\u5dee\u5f02\u8f83\u5927\uff0c\u5176\u4e2d\uff08111\uff09\u9762\u7684\u6d3b\u6027\u6700\u9ad8\uff0c\u5176\u6b21\u662f\uff08110\uff09\u9762\uff0c\u800c\uff08100\uff09\u9762\u5728\u5ba4\u6e29\u4e0b\u51e0\u4e4e\u6ca1\u6709\u6d3b\u6027\u3002<\/p>\n

\"\"<\/p>\n

Figure 1.<\/strong> Transmission electron microscope (TEM) images of CeO2<\/sub> (a) cube, (b) rod, (c) octa., and their corresponding high-resolution TEM images (row below). (d) Time-dependent yield of 2-PA in 2-Cp hydrolysis over CeO2<\/sub> shapes with equal tested weight (8 mg for each shape) and surface area (10.6 mg for cube, 3.6 mg for rod, and 8 mg for octa.) at room temperature. (e) Corresponding first-order rate constants.<\/p>\n

\u53cd\u5e94\u52a8\u529b\u5b66\u7814\u7a76\u8868\u660e\uff0c\u5728\u4e0d\u540c\u6e29\u5ea6\u4e0b\uff0c\u4e09\u79cdCeO2<\/sub>\u7684\u53cd\u5e94\u6d3b\u6027\u4ee5\u53ca\u901f\u7387\u5e38\u6570\uff08k\uff09\u7684\u8d8b\u52bf\u5747\u4e3a\uff08111\uff09>\uff08110\uff09>\uff08100\uff09\uff0c\u4f46\u5b83\u4eec\u5728Ea\u4e0a\u7684\u5dee\u5f02\u4e0d\u5927\uff0c\u8fd9\u4e00\u70b9\u65e0\u6cd5\u5145\u5206\u89e3\u91ca\u4e09\u8005\u6d3b\u6027\u7684\u663e\u8457\u5dee\u522b\uff0c\u8868\u660e\u5f88\u53ef\u80fd\u5b58\u5728\u5176\u4ed6\u56e0\u7d20\u3002<\/p>\n

\"\"<\/p>\n

Figure <\/strong>2<\/strong>.<\/strong> Temperature-dependent yield of 2-PA over CeO2<\/sub> shapes with equal tested surface area at (a) 40 \u00b0C, (b) 50 \u00b0C, (c) 60 \u00b0C, and (d) 70 \u00b0C. Comparison of their respective (e) k constant and (f) activation energy.<\/p>\n

EPR\u88ab\u7528\u4e8e\u786e\u8ba4\u50ac\u5316\u5242\u8868\u9762\u662f\u5426\u5b58\u5728\u6c27\u7a7a\u4f4d\u3002\u901a\u5e38\uff0cg = 2.00\u5904\u7684\u4fe1\u53f7\u4e0e\u6c27\u7a7a\u4f4d\u76f8\u5173\u8054\uff0c\u4f46\u4e09\u79cdCeO2<\/sub>\u7684EPR\u56fe\u8c31\u4e2d\u5747\u672a\u89c2\u5bdf\u5230\u8be5\u4fe1\u53f7\uff0c\u8fd9\u8868\u660e\u8868\u9762\u6c27\u7a7a\u4f4d\u5bf9\u5176\u6d3b\u6027\u51e0\u4e4e\u6ca1\u6709\u5f71\u54cd\u3002\u5728XPS\u7684Ce3d<\/sub>\u8c31\u56fe\u4e2d\uff0c\u4e09\u8005\u7684Ce3+<\/sup>\/Ce4+<\/sup>\u6bd4\u7387\u76f8\u8fd1\u3002\u5728O1s<\/sub>\u8c31\u56fe\u4e2d\uff0c\uff08111\uff09\u548c\uff08100\uff09\u9762\u5177\u6709\u76f8\u4f3c\u6570\u91cf\u7684\u8868\u9762\u6c27\uff08OS<\/sub>\uff09\u548c\u8868\u9762\u7f9f\u57fa\uff08OH<\/sub>\uff09\uff0c\u5374\u8868\u73b0\u51fa\u5de8\u5927\u7684\u6d3b\u6027\u5dee\u5f02\uff1b\u800c\u62e5\u6709\u6700\u591aOS<\/sub>\u548cOH<\/sub>\u7684\uff08110\uff09\u9762\u4ec5\u5448\u73b0\u51fa\u4e2d\u7b49\u6d3b\u6027\u3002\u56e0\u6b64\uff0c\u6211\u4eec\u53d1\u73b0\u5f88\u96be\u901a\u8fc7\u8fd9\u4e9b\u6574\u4f53\u6027\u8d28\u6765\u89e3\u91ca\u4e0d\u540c\u6676\u9762\u7684\u6d3b\u6027\u5dee\u5f02\u3002<\/p>\n

\"\"<\/p>\n

Figure <\/strong>3<\/strong>.<\/strong> (a) EPR, (b) XPS Ce3d<\/sub>, (c) XPS O1s<\/sub>, and (d) Raman spectra of CeO2<\/sub> shapes.<\/p>\n

DFT\u7ed3\u679c\u8868\u660e\uff0c\u7531\u4e8e\u4e0d\u540c\u7684Ce\u4f4d\u70b9\u8ddd\u79bb\uff0c2-Cp\u5728\u4e09\u79cd\u8868\u9762\u5c55\u73b0\u51fa\u4e0d\u540c\u7684\u5438\u9644\u6784\u578b\u3002\u5728\uff08100\uff09\u9762\uff0c\u672a\u80fd\u89c2\u5bdf\u52302-Cp\u7684\u5421\u5576-N\u548c\u6c30\u57fa-N\u4e4b\u95f4\u7684\u5438\u9644\u534f\u540c\u6548\u5e94\u3002\u800c\u5728\uff08110\uff09\u9762\u4e0a\uff0c2-Cp\u5b58\u5728\u591a\u79cd\u4e0d\u540c\u7684\u5438\u9644\u6784\u578b\u3002\u5176\u4e2d\uff0c\u90e8\u52062-Cp\u8868\u73b0\u4e3a\u534f\u540c\u5438\u9644\uff0c\u800c\u6240\u6709\uff08111\uff09\u9762\u4e0a\u76842-Cp\u5747\u4e3a\u534f\u540c\u5438\u9644\u3002<\/p>\n

\"\"<\/p>\n

Figure <\/strong>4<\/strong>.<\/strong> (a) The analysis of distances between N atoms in 2-Cp and Ce sites on CeO2<\/sub> surfaces. The adsorption configuration and energy of 2-Cp on (b) (100), (c) (110), (d) (111) surfaces with side (left) and top (right) views.<\/p>\n

\u7136\u800c\uff0c2-Cp\u7684\u5438\u9644\u80fd\uff08Ead<\/sub>\uff09\u8d8b\u52bf\u4e0e\u8868\u9762\u6d3b\u6027\u76f8\u53cd\uff0c\u8868\u660e2-Cp\u7684\u5438\u9644\u5e76\u975e\u5f71\u54cd\u6d3b\u6027\u7684\u5173\u952e\u6b65\u9aa4\u3002\u4e0e\u8def\u6613\u65af\u9178\uff08Lewis acid\uff09\u50ac\u5316\u673a\u5236\u4e0d\u540c\uff0cTamura\u7b49\u4eba\u63d0\u51fa\u4e00\u79cd\u65b0\u7684\u53cd\u5e94\u8def\u5f84\uff0c\u5373CeO2<\/sub>\u8868\u9762\u6676\u683c\u6c27\uff08Olattice<\/sub>\uff09\u5bf92-Cp\u7684\u6c30\u57fa-C\u8fdb\u884c\u4eb2\u6838\u653b\u51fb\u3002\u5728\uff08100\uff09\u9762\u4e0a\uff0c2-Cp\u7684\u6c34\u89e3\u4e0d\u80fd\u901a\u8fc7\u8fd9\u4e00\u8def\u5f84\u5b9e\u73b0\uff0c\u8fd9\u53ef\u80fd\u662f\u7531\u4e8eOlattice<\/sub>\u548c\u6c30\u57fa-C\u4e4b\u95f4\u7684\u8ddd\u79bb\u8f83\u8fdc\u4ee5\u53ca\u62ac\u5347Olattice<\/sub>\u6240\u9700\u7684\u80fd\u91cf\u8f83\u9ad8\u3002\u5bf9\u4e8e\uff08110\uff09\u9762\uff0cOlattice<\/sub>\u80fd\u591f\u8fdb\u884c\u4eb2\u6838\u653b\u51fb\uff0c\u4f46\u7531\u4e8eOlattice<\/sub>\u62ac\u5347\u7684\u8ddd\u79bb\u6709\u9650\uff0c\u6d3b\u5316\u76842-Cp\u5448\u503e\u659c\u6784\u578b\uff0c\u8fd9\u53ef\u80fd\u4f1a\u5bf9\u540e\u7eed\u5176\u4ed62-Cp\u7684\u6d3b\u5316\u9020\u6210\u7a7a\u95f4\u4f4d\u963b\uff0c\u4ece\u800c\u9650\u5236\u6709\u6548\u6d3b\u5316\u76842-Cp\u7684\u6570\u91cf\u3002\u5728\uff08111\uff09\u9762\u4e0a\uff0c2-Cp\u540c\u6837\u80fd\u591f\u901a\u8fc7\u8fd9\u4e00\u8def\u5f84\u8fdb\u884c\u6c34\u89e3\u3002\u533a\u522b\u5728\u4e8e\uff0c\u6d3b\u5316\u76842-Cp\u4fdd\u6301\u76f4\u7acb\u6784\u578b\uff0c\u5e76\u4e14\u7531\u4e8e\uff08111\uff09\u9762\u4e0aCe\u4f4d\u70b9\u7684\u5bc6\u96c6\u6392\u5217\uff0c\u76f8\u8f83\u4e8e\uff08110\uff09\u9762\uff0c\u524d\u8005\u80fd\u591f\u6d3b\u5316\u66f4\u591a\u76842-Cp\u3002Bader\u7535\u8377\u7ed3\u679c\u8868\u660e\uff0c\u57282-Cp\u7684\u5438\u9644\u548c\u6d3b\u5316\u8fc7\u7a0b\u4e2d\uff0c\u5421\u5576-N\u548c\u5421\u5576-C\u7684Bader\u7535\u8377\u53d8\u5316\u5fae\u5c0f\u3002\u76f8\u6bd4\u4e4b\u4e0b\uff0c\u6c30\u57fa-C\u7684\u7535\u5b50\u5bc6\u5ea6\u5728\u53d7\u5230Olattice<\/sub>\u7684\u4eb2\u6838\u653b\u51fb\u540e\u663e\u8457\u4e0b\u964d\uff0c\u8fd9\u4e0d\u4ec5\u589e\u5f3a\u4e86\u6c30\u57fa-C\u7684\u9178\u6027\uff0c\u4ee5\u4fbf\u8fdb\u884c\u968f\u540e\u7684\u6c34\/\u6c22\u6c27\u5316\u7269\u7684\u4eb2\u6838\u653b\u51fb\uff0c\u8fd8\u5bfc\u81f4\u6c30\u57fa-N\u7684\u7535\u5b50\u5bc6\u5ea6\u589e\u52a0\u3002<\/p>\n

\"\"<\/p>\n

Figure <\/strong>5<\/strong>.<\/strong> (a) Typical Lewis acid-catalyzed nitrile hydrolysis and (b) the proposed activation of the adsorbed 2-Cp by CeO2<\/sub> and its facilitated hydrolysis. The nucleophilic addition of the surface Olattice<\/sub> to the cyano-C atom of the adsorbed 2-Cp on (c) (110) and (d) (111) surfaces. The Bader charge analysis of (e) 2-Cp and the adsorbed 2-Cp before and after activation on (f) (110) and (g) (111) surfaces.<\/p>\n

\u6d4b\u8bd5\u4e86\u4e09\u79cd\u5f62\u8c8c\u7684CeO2<\/sub>\u5bf9 DMC\u5408\u6210\u53cd\u5e94\u7684\u50ac\u5316\u6d3b\u6027\uff0c\u53cd\u5e94\u6d3b\u6027\u987a\u5e8f\u4e3a\uff08111\uff09>\uff08110\uff09>\uff08100\uff09\u3002\u5728\u52a0\u51652-Cp\u540e\uff0cDMC\u7684\u4ea7\u91cf\u5747\u6709\u63d0\u5347\uff0c\u4e14\u6d3b\u6027\u987a\u5e8f\u4fdd\u6301\u4e0d\u53d8\u3002\u5176\u4e2d\uff0c\uff08111\uff09\u9762\u7684DMC\u4ea7\u91cf\u589e\u52a0\u7ea640\u500d\uff0c\u8fdc\u9ad8\u4e8e\u5176\u4ed6\u8868\u9762\u3002\u6b64\u5916\uff0c\u5728\u52a0\u51652-Cp\u540e\uff0cEa\u53d8\u5316\u4e0d\u5927\uff0c\u4e142-PA\u7684\u4ea7\u91cf\u4e0eDMC\u63a5\u8fd1\uff0c\u8868\u660eDMC\u4ea7\u91cf\u7684\u663e\u8457\u589e\u52a0\u662f\u7531\u4e8e2-Cp\u7684\u6c34\u89e3\u53bb\u9664\u4e86\u53cd\u5e94\u4e2d\u4ea7\u751f\u7684\u6c34\uff0c\u4f7f\u5f97\u53cd\u5e94\u5e73\u8861\u5411\u53f3\u79fb\u52a8\u3002<\/p>\n

\"\"<\/p>\n

Figure <\/strong>6<\/strong>.<\/strong> (a) The direct DMC synthesis catalyzed by CeO2<\/sub> shapes in the absence\/presence of 2-Cp at 140 \u00b0C, (b) the production of 2-PA during the direct DMC synthesis with 2-Cp, and (c) the corresponding EA<\/sub>.<\/p>\n

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

\u8be5\u5de5\u4f5c\u6df1\u5165\u7814\u7a76\u4e86\u4e0d\u540c\u6676\u9762\u7684CeO2<\/sub>\u57282-Cp\u6c34\u89e3\u4e2d\u7684\u4f5c\u7528\u3002\u5b9e\u9a8c\u7ed3\u679c\u8868\u660e\uff0c\u4e0d\u540c\u6676\u9762\u7684Ce\u4f4d\u70b9\u7684\u914d\u4f4d\u7ed3\u6784\u4f1a\u5f71\u54cd2-Cp\u5728\u50ac\u5316\u5242\u8868\u9762\u4e0a\u7684\u5438\u9644\u6784\u578b\uff0c\u4ece\u800c\u4f7f\u5f97CeO2<\/sub>\u57282-Cp\u6c34\u89e3\u4e2d\u5c55\u73b0\u51fa\u6676\u9762\u4f9d\u8d56\u6027\u3002\u5728\uff08100\uff09\u9762\u4e0a\uff0c2-Cp\u4e0d\u80fd\u534f\u540c\u5438\u9644\uff0c\u5bfc\u81f42-Cp\u7684\u6c34\u89e3\u53ea\u80fd\u901a\u8fc7\u8def\u6613\u65af\u9178\uff08Lewis acid\uff09\u6d3b\u5316\u9014\u5f84\uff0c\u8fd9\u4e00\u8def\u5f84\u9700\u8981\u7684\u8f83\u9ad8Ea\uff0c\u56e0\u6b64\u8be5\u8868\u9762\u6d3b\u6027\u8f83\u4f4e\u30022-Cp\u5728\uff08111\uff09\u9762\u548c\uff08110\uff09\u9762\u4e0a\u5b58\u5728\u534f\u540c\u5438\u9644\uff0c\u4f46\u540e\u8005\u7531\u4e8e\u7a7a\u95f4\u4f4d\u963b\u7684\u5b58\u5728\uff0c\u80fd\u540c\u65f6\u5438\u9644\u76842-Cp\u6570\u91cf\u5c11\u4e8e\u524d\u8005\uff0c\u9020\u6210\u4e86\u4e24\u8005\u7684\u6d3b\u6027\u5dee\u5f02\u3002\u56e0\u6b64\uff0c\u8fd9\u9879\u5de5\u4f5c\u8868\u660e\uff0c\u901a\u8fc7\u8c03\u63a7\u50ac\u5316\u5242\u8868\u9762\u6d3b\u6027\u4f4d\u70b9\u7684\u914d\u4f4d\u7ed3\u6784\uff0c\u53ef\u4ee5\u6539\u53d8\u53cd\u5e94\u7269\u7684\u5438\u9644\u6784\u578b\u3002<\/p>\n

\u539f\u6587\u8be6\u60c5\uff1a<\/strong>Tian, Linyuan, et al. “Unveiling the Pivotal Role of Ce Coordination Structures and Their Surface Arrangements in Governing 2-Cyanopyridine Hydrolysis for Direct Dimethyl Carbonate Synthesis from CO2 and Methanol.”\u00a0ACS Catalysis<\/em>\u00a014 (2024): 16861-16871.<\/p>\n

https:\/\/pubs.acs.org\/doi\/10.1021\/acscatal.4c04639<\/a><\/p>\n

\u672c\u6587\u7531buf.xiao\u4f9b\u7a3f<\/p>\n","protected":false},"excerpt":{"rendered":"

\u4e00\u3001\u3010\u5bfc\u8bfb\u3011 \u78b3\u9178\u4e8c\u7532\u916f\uff08DMC\uff09\u4f5c\u4e3a\u4e00\u79cd\u91cd\u8981\u7684\u5316\u5de5\u539f\u6750\u6599\uff0c\u5728\u6eb6\u5242\u3001\u805a\u5408\u7269\u5408\u6210\u3001\u71c3\u6599\/\u7535\u6c60\u6dfb\u52a0\u5242\u7b49\u9886\u57df\u5177\u6709\u5e7f\u6cdb\u5e94\u7528\u3002\u7136\u800c\uff0c\u4f20\u7edf\u7684DMC\u751f\u4ea7\u65b9\u6cd5\u4f9d\u8d56\u4e8e\u4f7f\u7528\u5371\u9669\u548c\u6613…<\/p>\n","protected":false},"author":2,"featured_media":0,"comment_status":"open","ping_status":"closed","sticky":false,"template":"","format":"standard","meta":{"footnotes":""},"categories":[215],"tags":[],"class_list":["post-263251","post","type-post","status-publish","format-standard","hentry","category-jiedu"],"_links":{"self":[{"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/posts\/263251"}],"collection":[{"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/posts"}],"about":[{"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/types\/post"}],"author":[{"embeddable":true,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/users\/2"}],"replies":[{"embeddable":true,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=%2Fwp%2Fv2%2Fcomments&post=263251"}],"version-history":[{"count":2,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/posts\/263251\/revisions"}],"predecessor-version":[{"id":263261,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=\/wp\/v2\/posts\/263251\/revisions\/263261"}],"wp:attachment":[{"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=%2Fwp%2Fv2%2Fmedia&parent=263251"}],"wp:term":[{"taxonomy":"category","embeddable":true,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=%2Fwp%2Fv2%2Fcategories&post=263251"},{"taxonomy":"post_tag","embeddable":true,"href":"http:\/\/www.cailiaoniu.com\/index.php?rest_route=%2Fwp%2Fv2%2Ftags&post=263251"}],"curies":[{"name":"wp","href":"https:\/\/api.w.org\/{rel}","templated":true}]}}