{"id":35387,"date":"2020-10-15T08:00:58","date_gmt":"2020-10-15T00:00:58","guid":{"rendered":"\/\/www.gsbet888.com\/?p=35387"},"modified":"2020-10-14T14:40:02","modified_gmt":"2020-10-14T06:40:02","slug":"14-ni%e8%bf%81%e7%a7%bb%e5%ae%9e%e7%8e%b0%e8%bf%9c%e7%a8%8bcsp2-h%e9%94%ae%e4%b8%8eco2%e7%9a%84%e7%be%a7%e5%9f%ba%e5%8c%96%e5%8f%8d%e5%ba%94","status":"publish","type":"post","link":"\/\/www.gsbet888.com\/%e5%8c%96%e5%ad%a6%e6%9d%82%e8%ae%b0\/recentpaper\/2020\/10\/14-ni%e8%bf%81%e7%a7%bb%e5%ae%9e%e7%8e%b0%e8%bf%9c%e7%a8%8bcsp2-h%e9%94%ae%e4%b8%8eco2%e7%9a%84%e7%be%a7%e5%9f%ba%e5%8c%96%e5%8f%8d%e5%ba%94.html","title":{"rendered":"1,4-Ni\u8fc1\u79fb\u5b9e\u73b0\u8fdc\u7a0bC(sp2)-H\u952e\u4e0eCO2\u7684\u7fa7\u57fa\u5316\u53cd\u5e94"},"content":{"rendered":"<p>\u672c\u6587\u4f5c\u8005\uff1aChemBoy<\/p>\n<h4>\u5bfc\u8bfb<\/h4>\n<p>\u6700\u8fd1\uff0c\u897f\u73ed\u7259\u52a0\u6cf0\u7f57\u5c3c\u4e9a\u5316\u5b66\u7814\u7a76\u6240\u7684Ruben Martin\u8bfe\u9898\u7ec4\u6210\u529f\u5229\u7528\u7b2c\u4e00\u4f8b[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\uff0c\u5b9e\u73b0\u4e86\u8fdc\u7a0b\u82b3\u70c3C(sp<sup>2<\/sup>)-H\u952e\u4e0eCO<sub>2<\/sub>\u7684\u7fa7\u57fa\u5316\u53cd\u5e94\u3002\u8be5\u53cd\u5e94\u4f5c\u4e3a\u7b2c\u4e00\u4f8b\u50ac\u5316[1,4]-Ni\u8fc1\u79fb\u53cd\u5e94\uff0c\u4e3a\u954d\u50ac\u5316\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u7684\u9886\u57df\u5f00\u8f9f\u4e86\u4e00\u6761\u65b0\u7684\u8def\u5f84\u3002\u540c\u65f6\uff0c\u4e5f\u4e3a\u8fdc\u7a0bC(sp<sup>2<\/sup>)-H\u952e\u4e0a\u5f15\u5165\u4eb2\u7535\u4f53\u63d0\u4f9b\u4e00\u4e2a\u65b0\u7684\u5e73\u53f0\u3002\u8be5\u7814\u7a76\u5de5\u4f5c\u53d1\u8868\u5728JACS\u4e0a\uff1a<\/p>\n<blockquote><p>\u201cRemote sp<sup>2<\/sup> C\u2212H Carboxylation via Catalytic 1,4-Ni Migration with CO<sub>2<\/sub>\u201d<\/p>\n<p>Marino Borjesson, Daniel Janssen-Muller, Basudev Sahoo, Yaya Duan, Xueqiang Wang, and Ruben Martin<sup>*<\/sup><\/p>\n<p><em>J. Am. Chem. Soc. <\/em><strong>2020<\/strong>,<em> 142, <\/em>16234<em>. <\/em>DOI: <a href=\"https:\/\/doi.org\/10.1021\/jacs.0c08810\">10.1021\/jacs.0c08810<\/a><\/p><\/blockquote>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35399 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1.jpg\" alt=\"\" width=\"919\" height=\"422\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1.jpg 919w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1-300x138.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1-680x312.jpg 680w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1-768x353.jpg 768w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-1-1-370x170.jpg 370w\" sizes=\"(max-width: 919px) 100vw, 919px\" \/><\/a><\/p>\n<h4><strong>\u524d\u8a00<\/strong><\/h4>\n<p>\u8fd1\u5e74\u6765\uff0c\u5df2\u62a5\u9053\u591a\u79cd\u5173\u4e8e\u82b3\u57fa\uff08\u62df\uff09\u5364\u5316\u7269\u4e0eCO<sub>2<\/sub>\u7684\u50ac\u5316\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u5408\u6210\u82ef\u7532\u9178\u53cd\u5e94\u7684\u8bbe\u8ba1\u4e0e\u53d1\u5c55\uff0c\u5176\u4e2d\u82ef\u7532\u9178\u4f5c\u4e3a\u751f\u7269\u6d3b\u6027\u5206\u5b50\u4e2d\u7684\u91cd\u8981\u90e8\u5206\u3002\u5c3d\u7ba1\u8be5\u9886\u57df\u5df2\u7ecf\u5230\u8fbe\u4e86\u8f83\u9ad8\u7684\u6c34\u5e73\uff0c\u4f46\u662f\u5728CO<sub>2<\/sub>\u63d2\u5165\u524d\u9700\u8981\u5bf9\u76ee\u6807C(sp<sup>2<\/sup>)\u53cd\u5e94\u4f4d\u70b9\u8fdb\u884c\u9884\u5b98\u80fd\u56e2\u5316\uff08Scheme 1, path a\uff09<sup>[1]<\/sup>\u3002\u6beb\u65e0\u7591\u95ee\uff0c\u5bfb\u6c42\u4e00\u79cd\u50ac\u5316\u7684C(sp<sup>2<\/sup>)-H\u952e\u76f4\u63a5\u7fa7\u57fa\u5316\u7684\u65b9\u6cd5\uff08Scheme 1, path b\uff09<sup>[2]<\/sup>\uff0c\u9664\u4e86\u5728\u6982\u5ff5\u548c\u5b9e\u7528\u6027\u65b9\u9762\uff0c\u5bf9\u5316\u5b66\u5f00\u53d1\u90fd\u662f\u6709\u4ef7\u503c\u7684\u52aa\u529b\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35400 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1.jpg\" alt=\"\" width=\"937\" height=\"510\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1.jpg 937w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1-300x163.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1-680x370.jpg 680w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-2-1-768x418.jpg 768w\" sizes=\"(max-width: 937px) 100vw, 937px\" \/><\/a><\/p>\n<p>\u53d7Fujiwara\u62a5\u9053\u7684\u5316\u5b66\u8ba1\u91cfPd\u914d\u5408\u7269\u8fd9\u4e00\u5f00\u521b\u6027\u5de5\u4f5c\u7684\u542f\u53d1<sup>[3]<\/sup>\uff0c\u51fa\u73b0\u4e86\u4e00\u4e9b\u91cd\u8981\u7684\u50ac\u5316\u9178\u6027C(sp<sup>2<\/sup>)-H\u952e<sup>[4<\/sup>]\u6216\u5bfc\u5411\u57fa\u5bfc\u5411\u7684C(sp<sup>2<\/sup>)-H\u952e\u76f4\u63a5\u7fa7\u57fa\u5316\u53cd\u5e94\u65b9\u6cd5\u7684\u62a5\u9053(Scheme 1, bottom)<sup>[5]<\/sup>\u3002\u7136\u800c\uff0c\u5bf9\u4e8e\u975e\u9178\u6027C(sp<sup>2<\/sup>)-H\u952e\u7684\u76f4\u63a5\u7fa7\u57fa\u5316\uff0c\u5728\u6ca1\u6709\u5bfc\u5411\u57fa\u56e2\u5b58\u5728\u7684\u60c5\u51b5\u4e0b\uff0c\u4f1a\u51fa\u73b0\u4f4d\u7f6e\u9009\u62e9\u6027\u95ee\u9898\uff0c\u5e76\u4e14\u9700\u8981\u4f7f\u7528\u8d35\u91d1\u5c5e\u6216\u5316\u5b66\u8ba1\u91cf\u7684\u6709\u673a\u91d1\u5c5e\u8bd5\u5242\uff08Scheme 1, bottom left\uff09<sup>[6]<\/sup>\u3002\u8fd9\u4e9b\u7ed3\u679c\u8ba9\u6709\u673a\u5316\u5b66\u5bb6\u4eec\u610f\u8bc6\u5230\uff0c\u65e0\u9700\u8d35\u91d1\u5c5e\u6216\u6709\u673a\u91d1\u5c5e\u8bd5\u5242\u8fdb\u884c\u7684\u50ac\u5316C(sp<sup>2<\/sup>)-H\u7fa7\u57fa\u5316\u7b56\u7565\u53ef\u80fd\u4f1a\u4e3aC(sp<sup>2<\/sup>)-H\u952e\u5b98\u80fd\u56e2\u5316\u4e0e\u7fa7\u57fa\u5316\u63d0\u4f9b\u65b0\u7684\u57fa\u7840\u77e5\u8bc6\u3002\u53d7\u6b64\u542f\u53d1\uff0c\u4f5c\u8005\u8bbe\u60f3\u662f\u5426\u53ef\u901a\u8fc7\u57fa\u4e8e\u4f4d\u7f6e\u9009\u62e9\u6027\u7684[1,4]-Ni\u8fc1\u79fb<sup>[7]<\/sup>\u7684\u4e32\u8054\u8fc7\u7a0b\u5b9e\u73b0CO<sub>2<\/sub>\u63d2\u5165\u8fdc\u7a0bC(sp<sup>2<\/sup>)-H\u952e\u7684\u53cd\u5e94\uff08Scheme 2\uff09\u3002\u4f5c\u8005\u5728\u5f00\u59cb\u7814\u7a76\u4e4b\u524d\uff0c\u8fd9\u79cd\u7b56\u7565\u80fd\u5426\u6210\u529f\u672a\u77e5\uff0c\u56e0\u4e3a\u6709\u4ee5\u4e0b\u4e24\u70b9\u539f\u56e0\uff1a\uff081\uff09\u76ee\u524d\uff0c\u5728\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u4e2d\u672a\u51fa\u73b0\u50ac\u5316\u7684[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u7684\u62a5\u9053\uff1b\uff082\uff09\u5728\u53cd\u5e94\u4e2d\u7531\u4e8eC(sp<sup>3<\/sup>)-Br\u952e\u4e0e\u7094\u57fa\u6d3b\u6cfc\u53cd\u5e94\u4f4d\u70b9\u7684\u5b58\u5728\uff0c\u4f1a\u9047\u5230\u4f4d\u7f6e\u9009\u62e9\u6027\u7684\u95ee\u9898<sup>[8]<\/sup>\u3002\u5982\u679c\u8be5\u8bbe\u60f3\u80fd\u591f\u6210\u529f\uff0c\u8fd9\u5c06\u6210\u4e3a\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u9886\u57df\u7684\u91cd\u5927\u7a81\u7834\uff0c\u53ef\u5b9e\u73b0\u5176\u4ed6\u65b9\u6cd5\u4e0d\u80fd\u5b9e\u73b0\u7684C(sp<sup>2<\/sup>)-H\u952e\u529f\u80fd\u5316\u7684\u53cd\u5e94\uff0c\u4ece\u800c\u4f5c\u4e3a\u4e00\u79cd\u65b0\u578b\u53cd\u5e94\u6a21\u5f0f\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35401 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1.jpg\" alt=\"\" width=\"936\" height=\"481\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1.jpg 936w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1-300x154.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1-680x349.jpg 680w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-3-1-768x395.jpg 768w\" sizes=\"(max-width: 936px) 100vw, 936px\" \/><\/a><\/p>\n<h4><strong>\u53cd\u5e94\u6761\u4ef6\u4f18\u5316<\/strong><\/h4>\n<p>\u9996\u5148\uff0c\u4f5c\u8005\u4ee5\u5316\u5408\u7269<strong>1a<\/strong>\u4f5c\u4e3a\u6a21\u677f\u5e95\u7269\u3001\u4ee5CO<sub>2<\/sub>\u4e3a\u7fa7\u57fa\u6e90\u5bf9\u53cd\u5e94\u6761\u4ef6\u8fdb\u884c\u7b5b\u9009\uff08Table 1\uff09\u3002\u4e0d\u51fa\u6240\u6599\uff0c\u5f53\u4f7f\u7528\u4ee5\u524d\u62a5\u9053\u7684\u82b3\u57fa\u5364\u5316\u7269\u4e0eCO<sub>2<\/sub>\u7684\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u53cd\u5e94\u6761\u4ef6\u65f6<sup>[9]<\/sup>\uff0c\u4ec5\u89c2\u5bdf\u5230\u5fae\u91cf\u7684\u76ee\u6807\u4ea7\u7269<strong>2a<\/strong>\uff0c\u4e3b\u8981\u662f\u751f\u6210\u4e86CO<sub>2<\/sub>\u4e0e\u7094\u57fa\u53cd\u5e94\u7684\u526f\u4ea7\u7269<strong>2a\u2019<\/strong>\u3002\u5728\u5bf9\u53cd\u5e94\u53c2\u6570\u8fdb\u884c\u4f18\u5316\u540e\uff0c\u53d1\u73b0NiBr<sub>2<\/sub>.diglyme\u3001<strong>L5<\/strong>\u4e0eMn<sub>89<\/sub>Cr<sub>11<\/sub>\u7684\u7ec4\u5408\u4f7f\u7528\u662f\u53cd\u5e94\u6210\u529f\u7684\u5173\u952e\uff0c\u80fd\u4ee577%\u7684\u4ea7\u7387\u4e0e\u4f18\u79c0\u7684\u4f4d\u7f6e\u9009\u62e9\u6027\uff08<strong>2a:2a\u2019<\/strong>=94:6\uff09\u751f\u6210\u76ee\u6807\u4ea7\u7269<strong>2a<\/strong>(Table 1, entry 1)\u3002\u968f\u540e\uff0c\u4f5c\u8005\u5bf9\u914d\u4f53\u6838\u5fc3\u9aa8\u67b62,2-\u8054\u5421\u5576\u7684\u7535\u6027\u6216\u4f4d\u963b\u8fdb\u884c\u8c03\u6574\uff0c\u53d1\u73b0\u5bf9\u53cd\u5e94\u6d3b\u6027\u6709\u4e0d\u53ef\u5ffd\u89c6\u7684\u5f71\u54cd\uff08Table 1, entries 2-5\uff09\uff1b\u663e\u8457\u5730\uff0c\u4f7f\u7528\u5176\u4ed6\u7c7b\u91d1\u5c5e\u8fd8\u539f\u5242\u66ff\u4ee3Mn<sub>89<\/sub>Cr<sub>11<\/sub>\u65f6\uff0c\u53cd\u5e94\u7684\u4ea7\u7387\u4e0e\u9009\u62e9\u6027\u5747\u660e\u663e\u964d\u4f4e\uff08Table1, entries 6-8\uff09\uff1b\u5c3d\u7ba1\u6709\u4eba\u8ba4\u4e3aCr\u539f\u5b50\u7684\u5b58\u5728\u53ef\u80fd\u51b3\u5b9a\u4e86\u53cd\u5e94\u7684\u4f4d\u7f6e\u9009\u62e9\u6027\uff0c\u800centry 7\u4e0eentry 8\u8bc1\u660e\u7ed3\u679c\u5374\u76f8\u53cd\uff0c\u76ee\u524d\u4f5c\u8005\u5bf9Cr\u7684\u4f5c\u7528\u4e5f\u65e0\u6cd5\u89e3\u91ca\u3002\u63a5\u7740\u4f5c\u8005\u53d1\u73b0\u4f7f\u7528Ni(cod)<sub>2<\/sub>\u4f5c\u4e3a\u50ac\u5316\u5242\u6216DMSO\u66ff\u6362DMF\u4f5c\u4e3a\u6eb6\u5242\u65f6\uff08entry 9 and entry 10\uff09\uff0c\u5747\u65e0\u6cd5\u8fbe\u5230\u7406\u60f3\u7684\u7ed3\u679c\u3002\u7136\u800c\uff0c\u5f53\u4f7f\u7528\u5bf9\u7a7a\u6c14\u4e0e\u6e7f\u6c14\u7a33\u5b9a\u7684NiBr<sub>2<\/sub>(L5)<sub>2<\/sub>\u4f5c\u4e3a\u50ac\u5316\u5242\u65f6\uff0c\u80fd\u4ee5\u4f18\u79c0\u7684\u4ea7\u7387\u4e0e\u4f4d\u7f6e\u9009\u62e9\u6027\u751f\u6210\u76ee\u6807\u4ea7\u7269\uff0c\u4f5c\u8005\u4ee5\u6b64\u4e3a\u6700\u4f18\u53cd\u5e94\u6761\u4ef6\uff08Table 1, entry 11\uff09\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35402 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1.jpg\" alt=\"\" width=\"893\" height=\"875\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1.jpg 893w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1-300x294.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1-680x666.jpg 680w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-4-1-768x753.jpg 768w\" sizes=\"(max-width: 893px) 100vw, 893px\" \/><\/a><\/p>\n<h4><strong>\u5e95\u7269\u62d3\u5c55<\/strong><\/h4>\n<p>\u5728\u786e\u5b9a\u6700\u4f18\u53cd\u5e94\u6761\u4ef6\u540e\uff0c\u4f5c\u8005\u5bf9\u8be5\u53cd\u5e94\u7684\u5e95\u7269\u8303\u56f4\u8fdb\u884c\u63a2\u7d22\uff08Table 2\uff09\u3002\u4f5c\u8005\u53d1\u73b0\uff0c\u5e95\u7269\u7ed3\u6784\u4e2d\u542b\u6709\u786b\u919a(<strong>2d<\/strong>)\u3001\u7532\u6c27\u82b3\u70c3(<strong>2b<\/strong>)\u3001\u4e09\u6c1f\u7532\u57fa\u884d\u751f\u7269(<strong>2c<\/strong> and <strong>2i<\/strong>)\u6216\u6742\u73af\uff08<strong>2o<\/strong>\uff09\u65f6\uff0c\u53cd\u5e94\u5747\u80fd\u5b8c\u7f8e\u5730\u8fdb\u884c\u3002\u751a\u81f3\u82b3\u57fa\u5364\u5316\u7269\uff08<strong>2g<\/strong>, <strong>2h<\/strong> and <strong>2r<\/strong>\uff09\u6216\u6709\u673a\u787c\u5316\u7269\uff08<strong>2e<\/strong>\uff09\u4e5f\u80fd\u517c\u5bb9\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\u7094\u70c3\u90e8\u5206\u65e0\u8bba\u662f\u5927\u4f4d\u963b\u82b3\u57fa\uff08<strong>2m<\/strong>\uff09\u6216\u8102\u80aa\u70f7\u57fa\u53d6\u4ee3\uff08<strong>2j-l<\/strong>\uff09\u5e95\u7269\u4e5f\u80fd\u4ee5\u4f18\u79c0\u7684\u4ea7\u7387\u83b7\u5f97\u76ee\u6807\u4ea7\u7269\u3002\u65e0\u8bba\u662f\u7094\u70c3\u9aa8\u67b6\u4e0a\u7684\u4f4d\u963b\u56e0\u7d20\u8fd8\u662f\u60f0\u6027\u4e8c\u7ea7\u70f7\u57fa\u6eb4\u5316\u7269\uff08<strong>2p<\/strong> and<strong> 2q<\/strong>\uff09\u5747\u80fd\u4ee5\u8f83\u9ad8\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807C(sp<sup>2<\/sup>)-H\u952e\u7fa7\u57fa\u5316\u4ea7\u7269\u3002\u6709\u8da3\u7684\u662f\uff0c\u82b3\u73af\u4e0a\u5b58\u5728\u4e0d\u540c\u53d6\u4ee3\u57fa\u65f6\u4e5f\u4e0d\u80fd\u963b\u6b62[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u7684\u53d1\u751f\uff0c\u5c3d\u7ba1\u53cd\u5e94\u7684\u4ea7\u7387\u6bd4\u8f83\u4f4e\uff08<strong>2r<\/strong> and <strong>2s<\/strong>\uff09\uff1b\u6b64\u5916\uff0c\u901a\u8fc7Si\u539f\u5b50\u94fe\u63a5\u70f7\u57fa\u6eb4\u5316\u7269\u5c24\u5176\u91cd\u8981\uff0c\u4e5f\u80fd\u83b7\u5f97\u76ee\u6807\u7fa7\u9178\u4ea7\u7269\uff08<strong>2t-w<\/strong>\uff09\uff0c\u6240\u5f97\u7fa7\u9178\u4ea7\u7269\u53ef\u901a\u8fc7\u540e\u671f\u7684C-Si\u952e\u65ad\u88c2\u751f\u6210\u975e\u7a20\u73af\u7c7b\u5316\u5408\u7269\uff08Scheme 4, bottom\uff09\u3002<\/p>\n<p>\u5316\u5408\u7269<strong>2a-w<\/strong>\u7684\u6210\u529f\u5408\u6210\uff0c\u4f5c\u8005\u8ba4\u4e3a\u7b80\u5355\u70ef\u57fa\u5364\u5316\u7269\u4f5c\u4e3a\u5e95\u7269\u65f6\u5e94\u8be5\u4e5f\u80fd\u53d1\u751f\u7c7b\u4f3c\u7684[1,4]-Ni\u8fc1\u79fb\u7684\u8fdc\u7a0bC(sp<sup>2<\/sup>)-H\u952e\u7fa7\u57fa\u5316\u53cd\u5e94\u3002\u5982Scheme 3\u6240\u793a\uff0c\u4f5c\u8005\u5c06\u53cd\u5e94\u6eb6\u5242\u7531DMF\u6539\u4e3aDMA\u540e\uff0c\u5176\u4ed6\u6761\u4ef6\u4e0d\u53d8\uff0c\u53d1\u73b0\u65e0\u8bba\u662f\u70f7\u57fa\u53d6\u4ee3\u8fd8\u662f\u82b3\u57fa\u53d6\u4ee3\u7684\u70ef\u57fa\u6eb4\u5316\u7269\u5747\u80fd\u53d1\u751f\u76ee\u6807C(sp<sup>2<\/sup>)-H\u952e\u76f4\u63a5\u7fa7\u57fa\u5316\u751f\u6210\u76ee\u6807\u4ea7\u7269<strong>4a<\/strong>\uff08E\/Z=2.4\/1\uff09\u4e0e<strong>4b<\/strong>(E\/Z=3.3\/1), \u5c3d\u7ba1\u5e95\u7269<strong>3a<\/strong>\u4e0e<strong>3b<\/strong>\u5747\u4e3aE\/Z\u5f02\u6784\u4f53\u6df7\u5408\u7269\u3002\u5b9e\u9a8c\u7ed3\u679c\u8868\u660e\uff0c\u5e95\u7269\u4e0e\u50ac\u5316Ni(0)\u7269\u79cd\u53d1\u751f\u6c27\u5316\u52a0\u6210\u5f62\u6210\u7684Ni(II)\u7269\u79cd\u5728\u53d1\u751f[1,4]-Ni\u8fc1\u79fb\u6b65\u9aa4\u4e4b\u524d\u4f1a\u53d1\u751fE\/Z\u5f02\u6784\u5316\uff0c\u8fc7\u7a0b\u4e2d\u53ef\u80fd\u5b58\u5728\u5361\u5bbe\u7c7b\u4e2d\u95f4\u4f53<sup>[10]<\/sup>\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-5-1.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35403 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-5-1.jpg\" alt=\"\" width=\"736\" height=\"1031\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-5-1.jpg 736w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-5-1-214x300.jpg 214w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-5-1-680x953.jpg 680w\" sizes=\"(max-width: 736px) 100vw, 736px\" \/><\/a><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-66.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35407 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-66.jpg\" alt=\"\" width=\"751\" height=\"520\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-66.jpg 751w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-66-300x208.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-66-680x471.jpg 680w\" sizes=\"(max-width: 751px) 100vw, 751px\" \/><\/a><\/p>\n<h4><strong>\u884d\u751f\u5316\u7814\u7a76<\/strong><\/h4>\n<p>\u6b64\u5916\uff0c\u4f5c\u8005\u4e3a\u4e86\u8bc1\u660e[1,4]-Ni\u8fc1\u79fb\u6280\u672f\u7684\u5e94\u7528\u4ef7\u503c\uff0c\u5bf9\u7fa7\u57fa\u5316\u4ea7\u7269\u8fdb\u884c\u4e86\u4e00\u7cfb\u5217\u7684\u884d\u751f\u5316\u5e94\u7528\uff08Scheme 4\uff09\u3002\u7fa7\u9178<strong>2a<\/strong>\u6216<strong>2b<\/strong>\u5728\u4e24\u79cd\u4e0d\u540c\u7684\u53cd\u5e94\u6761\u4ef6\u4e0b\u80fd\u591f\u5408\u6210\u5f02\u8272\u6ee1\u916e\u6216\u82ef\u915e\u7c7b\u590d\u6742\u5206\u5b50\uff0c\u7fa7\u9178<strong>2a<\/strong>\u5728TFA( 10mol%)\u3001NBS\u5b58\u5728\u6761\u4ef6\u4e0b\u53d1\u751f\u6eb4\u5185\u916f\u5316\u4ee583%\u7684\u4ea7\u7387\u751f\u6210\u82ef\u915e\u7c7b\u5316\u5408\u7269<strong>5<\/strong>\uff0c\u800c\u5728H<sub>2<\/sub>SO<sub>4<\/sub>\u4f5c\u7528\u6761\u4ef6\u4e0b\u80fd\u4ee588%\u7684\u4ea7\u7387\u751f\u6210\u82ef\u915e\u7c7b\u5316\u5408\u7269<strong>6<\/strong>\uff1b\u76f8\u4f3c\u5730\uff0c<strong>2a<\/strong>\u5728PdCl(MeCN)<sub>2<\/sub>\u50ac\u5316\u4f5c\u7528\u4e0b\u80fd\u4ee588%\u7684\u4ea7\u7387\u83b7\u5f97\u5f02\u8272\u6ee1\u916e\u7c7b\u5316\u5408\u7269<strong>7<\/strong>\uff0c\u540c\u65f6<strong>2b<\/strong>\u5728H<sub>2<\/sub>SO<sub>4<\/sub>\u5b58\u5728\u6761\u4ef6\u4e0b\u80fd\u4ee562%\u7684\u4ea7\u7387\u83b7\u5f97\u5f02\u8272\u6ee1\u916e\u7c7b\u4f3c\u7269<strong>8<\/strong>(<em>dr<\/em> 4.2:1)\u3002\u91cd\u8981\u7684\u662f\uff0c\u5b58\u5728Si\u539f\u5b50\u7684\u7fa7\u9178<strong>2w<\/strong> \u5728TMSCHN<sub>2<\/sub>\u3001H<sub>2<\/sub>O<sub>2<\/sub>\u4f5c\u7528\u4e0b\u80fd\u591f\u53d1\u751fC-Si\u952e\u65ad\u88c2\u4ee543%\u7684\u4ea7\u7387\u83b7\u5f97\u591a\u7f9f\u57fa\u7fa7\u9178\u916f\u7c7b\u5316\u5408\u7269<strong>9<\/strong>\uff0c\u8fdb\u4e00\u6b65\u8bc1\u5b9e\u4e86\u8be5\u7fa7\u57fa\u5316\u53cd\u5e94\u65b9\u6cd5\u7684\u5b9e\u7528\u6027\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-7.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35405 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-7.jpg\" alt=\"\" width=\"740\" height=\"805\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-7.jpg 740w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-7-276x300.jpg 276w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-7-680x740.jpg 680w\" sizes=\"(max-width: 740px) 100vw, 740px\" \/><\/a><\/p>\n<h4><strong>\u53cd\u5e94\u673a\u7406\u63a2\u7d22<\/strong><\/h4>\n<p>\u6700\u540e\uff0c\u4f5c\u8005\u5bf9\u53cd\u5e94\u673a\u7406\u8fdb\u884c\u4e86\u521d\u6b65\u7814\u7a76(Scheme 5)\u3002\u9996\u5148\uff0c\u4f5c\u8005\u4ee5<strong>3c<\/strong>\u4f5c\u4e3a\u5e95\u7269\u8fdb\u884c\u4e86\u540c\u4f4d\u7d20\u6807\u8bb0\u7814\u7a76(Scheme 5, top)\uff0c<strong>3c<\/strong>\u5728\u6700\u4f73\u53cd\u5e94\u6761\u4ef6\u4e0b\u8fdb\u884c\u53cd\u5e94\u4ee545%\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807\u4ea7\u7269<strong>4c<\/strong>\uff0c\u5176\u4e2d<strong>4c<\/strong>\u7684\u70ef\u57fa\u4f4d\u7684\u6c18\u4ee3\u7387\u5927\u4e8e95%\uff0c\u8bc1\u660e\u5728CO<sub>2<\/sub>\u63d2\u5165\u76ee\u6807C(sp<sup>2<\/sup>)-H\u952e\u524d\u5728\u70ef\u57fa\u90bb\u4f4dC(sp<sup>2<\/sup>)-H\u952e\u4e0a\u53d1\u751f\u4e86[1,4]-Ni\u8fc1\u79fb\uff1b\u6709\u8da3\u7684\u662f\uff0c\u5bf9\u5316\u5408\u7269<strong>3d<\/strong>\u8fdb\u884c\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u53cd\u5e94\u65f6\uff0c\u53d1\u73b0\u4e86\u660e\u663e\u7684\u5206\u5b50\u5185\u52a8\u529b\u5b66\u540c\u4f4d\u7d20\u6548\u5e94\uff08K<sub>H<\/sub>\/K<sub>D<\/sub>=5:1; Scheme 5, top right\uff09\uff0c\u4f5c\u8005\u901a\u8fc7<strong>3a<\/strong>\u4e0e<strong>3c<\/strong>\u7684\u53cd\u5e94\u901f\u7387\u5bf9\u6bd4\u672a\u53d1\u73b0\u5206\u5b50\u95f4\u52a8\u529b\u5b66\u540c\u4f4d\u7d20\u6548\u5e94\u3002\u8fd9\u4e9b\u7ed3\u679c\u8868\u660e\uff0c\u5728\u53d1\u751f[1,4]-Ni\u8fc1\u79fb\u524d\u6216\u8fc1\u79fb\u540e\u5b58\u5728\u4e00\u4e2a\u51b3\u901f\u6b65\u9aa4\u3002\u5c3d\u7ba1\u5982\u6b64\uff0c\u4ecd\u4e0d\u77e5CO<sub>2<\/sub>\u63d2\u5165\u4e0e[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u662f\u53d1\u751f\u5728Ni(I)\u8fd8\u662fNi(II)\u91d1\u5c5e\u4e2d\u5fc3\u4e0a\u3002\u56e0\u800c\uff0c\u4f5c\u8005\u5c06\u6ce8\u610f\u529b\u8f6c\u79fb\u5230\u6c27\u5316\u52a0\u6210\u5f62\u6210\u7684\u70ef\u57fa\u6216\u82b3\u57fa\u954d\u91d1\u5c5e\u914d\u5408\u7269\u4e2d\u95f4\u7684\u5206\u79bb\u4e0a\uff08Scheme 5, bottom\uff09\u3002\u6709\u8da3\u7684\u662f\uff0c\u82b3\u57fa\uff08\u70ef\u57fa\uff09\u5364\u5316\u7269\u4e0eNi(cod)<sub>2<\/sub>\u548cTMEDA\u6216<strong>L2<\/strong>\u5728THF\u6eb6\u5242\u4e2d\u80fd\u53d1\u751f\u53cd\u5e94\u5206\u522b\u751f\u6210\u954d\u6709\u673a\u91d1\u5c5e\u7edc\u5408\u7269<strong>10<\/strong>\u4e0e<strong>11<\/strong>\u3002\u4f5c\u8005\u4ee5\u8fd9\u4e24\u79cd\u954d\u7edc\u5408\u7269\u4f5c\u4e3a\u53cd\u5e94\u7269\u8fdb\u884c\u7fa7\u57fa\u5316\u53cd\u5e94\u7814\u7a76\uff0c\u53d1\u73b0<strong>10<\/strong>\u4ec5\u5728<strong>L5<\/strong>\u5b58\u5728\u6761\u4ef6\u4e0b\u5c31\u80fd\u4e0eCO<sub>2<\/sub>\u53d1\u751f\u53cd\u5e94\u4ee549%\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807\u7fa7\u57fa\u5316\u4ea7\u7269<strong>4a<\/strong>, \u8bc1\u5b9e2,2\u2019-\u8054\u5421\u5576\u914d\u4f53\u5bf9\u53d1\u751f\u76ee\u6807\u7fa7\u57fa\u5316\u53cd\u5e94\u7684\u91cd\u8981\u6027\uff1b\u66f4\u91cd\u8981\u7684\u662f\uff0c<strong>10<\/strong>\u4e0e<strong>11<\/strong>\u5747\u80fd\u5728\u65e0\u5916\u52a0\u91d1\u5c5e\u8fd8\u539f\u5242\u5b58\u5728\u6761\u4ef6\u4e0b\u53d1\u751f\u7fa7\u57fa\u5316\u53cd\u5e94\u751f\u6210\u76ee\u6807\u4ea7\u7269<strong>4a<\/strong>, \u8fdb\u4e00\u6b65\u8bc1\u660e[1,4]-\u8fc1\u79fb\u8fc7\u7a0b\u7684\u5b58\u5728\u548cCO<sub>2<\/sub>\u7684\u63d2\u5165\u53d1\u751f\u5728Ni(II)\u91d1\u5c5e\u4e2d\u5fc3\u4e0a\u3002\u6211\u4eec\u4e0d\u80fd\u4f4e\u4f30\u8fd9\u4e00\u5b9e\u9a8c\u7ed3\u679c\uff0c\u56e0\u4e3a\u5b83\u6311\u6218\u4e86\u4e4b\u524d\u666e\u904d\u7684\u89c2\u70b9\uff0c\u5373CO<sub>2<\/sub>\u7684\u63d2\u5165\u4e0e[1,4]-\u8fc1\u79fb\u53d1\u751f\u5728Ni(I)\u91d1\u5c5e\u4e2d\u5fc3\u4e0a\u3002\u4ece\u800c\u4e3a\u50ac\u5316\u5242\u7684\u8bbe\u8ba1\u63d0\u4f9b\u4e86\u4e00\u79cd\u65b0\u7684\u601d\u8def\uff0c\u5c24\u5176\u662f\u5728\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u9886\u57df\u3002<\/p>\n<p><a href=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8.jpg\"><img loading=\"lazy\" decoding=\"async\" class=\"aligncenter wp-image-35406 size-full\" src=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8.jpg\" alt=\"\" width=\"909\" height=\"848\" srcset=\"https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8.jpg 909w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8-300x280.jpg 300w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8-680x634.jpg 680w, https:\/\/assets.www.gsbet888.com\/uploads\/2020\/10\/1-8-768x716.jpg 768w\" sizes=\"(max-width: 909px) 100vw, 909px\" \/><\/a><\/p>\n<h4>\u603b\u7ed3\u4e0e\u8bc4\u4ef7<\/h4>\n<p>Martin\u6559\u6388\u8bfe\u9898\u7ec4\u62a5\u9053\u4e86\u9996\u4f8b\u4ee5\u50ac\u5316\u76841,4-Ni\u8fc1\u79fb\u4f5c\u4e3a\u5de5\u5177\u4fc3\u4f7fCO<sub>2<\/sub>\u4e0e\u8fdc\u7a0bC(sp<sup>2<\/sup>)-H\u952e\u7684\u76f4\u63a5\u7fa7\u57fa\u5316\u53cd\u5e94\u65b9\u6cd5\uff0c\u8be5\u7b56\u7565\u65e0\u8bba\u662f\u5728\u7fa7\u57fa\u5316\u8fd8\u662f\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u9886\u57df\u5747\u672a\u88ab\u5176\u4ed6\u8bfe\u9898\u7ec4\u62a5\u9053\u8fc7\uff0c\u5e76\u4e14\u8be5\u65b9\u6cd5\u5177\u6709\u7cbe\u51c6\u7684\u5316\u5b66\u4e0e\u4f4d\u7f6e\u9009\u62e9\u6027\u3001\u53cd\u5e94\u6761\u4ef6\u6e29\u548c\u4e0e\u5b9e\u7528\u6027\u7684\u7279\u70b9\u3002<\/p>\n<h4>\u53c2\u8003\u6587\u732e<\/h4>\n<ul>\n<li>[1] Tortajada, A.; Julia-Hernandez, F.; Borjesson, M.; Moragas, T.; Martin, R. <em>Angew. Chem., Int. Ed.<\/em> <strong>2018<\/strong>, <em>57<\/em>, 15948.DOI: <a href=\"https:\/\/doi.org\/10.1002\/anie.201803186\">10.1002\/anie.201803186<\/a><\/li>\n<li>[2] Hong, J.; Li, M.; Zhang, J.; Sun, B.; Mo, F. ChemSusChem <strong>2019<\/strong>, <em>12<\/em>, 6. DOI: <a href=\"https:\/\/doi.org\/10.1002\/cssc.201802012\">10.1002\/cssc.201802012<\/a><\/li>\n<li>[3] Sugimoto, H.; Kawata, I.; Taniguchi, H.; Fujiwara, Y. <em>J. Organomet. Chem. <\/em><strong>1984<\/strong>, <em>266<\/em>, C44. DOI:<a href=\"https:\/\/doi.org\/10.1016\/0022-328X(84)80150-3\">10.1016\/0022-328X(84)80150-3<\/a><\/li>\n<li>[4] Zhang, L.; Cheng, J.; Ohishi, T.; Hou, Z.<em> Angew. Chem., Int. Ed.<\/em> <strong>2010<\/strong>, <em>49<\/em>, 8670. DOI:<a href=\"https:\/\/doi.org\/10.1002\/anie.201003995\">10.1002\/anie.201003995<\/a><\/li>\n<li>[5] Mizuno, H.; Takaya, J.; Iwasawa, N. <em>J. Am. Chem. Soc.<\/em> <strong>2011<\/strong>, <em>133<\/em>, 1251.DOI: <a href=\"https:\/\/doi.org\/10.1021\/ja109097z\">10.1021\/ja109097z<\/a><\/li>\n<li>[6] Suga, T.; Saitou, T.; Takaya, J.; Iwasawa, N.<em> Chem. Sci.<\/em> <strong>2017<\/strong>, <em>8<\/em>, 1454.DOI: <a href=\"https:\/\/doi.org\/10.1039\/c6sc03838g\">10.1039\/c6sc03838g<\/a><\/li>\n<li>[7] Ma, S.; Gu, Z. <em>Angew. Chem., Int. Ed.<\/em> <strong>2005<\/strong>, <em>44<\/em>, 7512. DOI: <a href=\"https:\/\/doi.org\/10.1002\/anie.200501298\">10.1002\/anie.200501298<\/a><\/li>\n<li>[8] (a) Julia-Hernandez, F.; Moragas, T.; Cornella, J.; Martin, R. <em>Nature<\/em> <strong>2017<\/strong>, <em>545<\/em>, 84.DOI: <a href=\"https:\/\/doi.org\/10.1038\/nature22316\">10.1038\/nature22316<\/a>. (b) Gaydou, M.; Moragas, T.; Julia-Hernandez, F.; Martin, R. \u00a0<em>J. Am. Chem. Soc.<\/em> <strong>2017<\/strong>, <em>139,<\/em> 12161.DOI: <a href=\"https:\/\/doi.org\/10.1021\/jacs.7b07637\">10.1021\/jacs.7b07637<\/a><\/li>\n<li>[9] Fujihara, T.; Nogi, K.; Xu, T.; Terao, J.; Tsuji, Y. <em>J. Am. Chem. Soc<\/em>. <strong>2012<\/strong>, <em>134<\/em>, 9106. DOI: <a href=\"https:\/\/doi.org\/10.1021\/ja303514b\">10.1021\/ja303514b<\/a><\/li>\n<li>[10] Liu, X.; Li, X.; Chen, Y.; Hu, Y.; Kishi, Y. <em>J. Am. Chem. Soc.<\/em> <strong>2012<\/strong>, <em>134<\/em>, 6136. DOI:<a href=\"https:\/\/doi.org\/10.1021\/ja302177z\">10.1021\/ja302177z<\/a><\/li>\n<\/ul>\n<p>\u672c\u6587\u7248\u6743\u5c5e\u4e8e<strong>\u00a0<a href=\"\/\/www.gsbet888.com\/\">Chem-Station\u5316\u5b66\u7a7a\u95f4<\/a>\uff0c<\/strong>\u00a0\u6b22\u8fce\u70b9\u51fb\u6309\u94ae\u5206\u4eab\uff0c\u672a\u7ecf\u8bb8\u53ef\uff0c\u8c22\u7edd\u8f6c\u8f7d\uff01<\/p>\n","protected":false},"excerpt":{"rendered":"\u672c\u6587\u4f5c\u8005\uff1aChemBoy \u5bfc\u8bfb \u6700\u8fd1\uff0c\u897f\u73ed\u7259\u52a0\u6cf0\u7f57\u5c3c\u4e9a\u5316\u5b66\u7814\u7a76\u6240\u7684Ruben Martin\u8bfe\u9898\u7ec4\u6210\u529f\u5229\u7528\u7b2c\u4e00\u4f8b[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\uff0c\u5b9e\u73b0\u4e86\u8fdc\u7a0b\u82b3\u70c3C(sp2)-H\u952e\u4e0eCO2\u7684\u7fa7\u57fa\u5316\u53cd\u5e94\u3002\u8be5\u53cd\u5e94\u4f5c\u4e3a\u7b2c\u4e00\u4f8b\u50ac\u5316[1,4]-Ni\u8fc1\u79fb\u53cd\u5e94\uff0c\u4e3a\u954d\u50ac\u5316\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u7684\u9886\u57df\u5f00\u8f9f\u4e86\u4e00\u6761\u65b0\u7684\u8def\u5f84\u3002\u540c\u65f6\uff0c\u4e5f\u4e3a\u8fdc\u7a0bC(sp2)-H\u952e\u4e0a\u5f15\u5165\u4eb2\u7535\u4f53\u63d0\u4f9b\u4e00\u4e2a\u65b0\u7684\u5e73\u53f0\u3002\u8be5\u7814\u7a76\u5de5\u4f5c\u53d1\u8868\u5728JACS\u4e0a\uff1a \u201cRemote sp2 C\u2212H Carboxylation via Catalytic 1,4-Ni Migration with CO2\u201d Marino Borjesson, Daniel Janssen-Muller, Basudev Sahoo, Yaya Duan, Xueqiang Wang, and Ruben Martin* J. Am. Chem. Soc. 2020, 142, 16234. DOI: 10.1021\/jacs.0c08810 \u524d\u8a00 \u8fd1\u5e74\u6765\uff0c\u5df2\u62a5\u9053\u591a\u79cd\u5173\u4e8e\u82b3\u57fa\uff08\u62df\uff09\u5364\u5316\u7269\u4e0eCO2\u7684\u50ac\u5316\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u5408\u6210\u82ef\u7532\u9178\u53cd\u5e94\u7684\u8bbe\u8ba1\u4e0e\u53d1\u5c55\uff0c\u5176\u4e2d\u82ef\u7532\u9178\u4f5c\u4e3a\u751f\u7269\u6d3b\u6027\u5206\u5b50\u4e2d\u7684\u91cd\u8981\u90e8\u5206\u3002\u5c3d\u7ba1\u8be5\u9886\u57df\u5df2\u7ecf\u5230\u8fbe\u4e86\u8f83\u9ad8\u7684\u6c34\u5e73\uff0c\u4f46\u662f\u5728CO2\u63d2\u5165\u524d\u9700\u8981\u5bf9\u76ee\u6807C(sp2)\u53cd\u5e94\u4f4d\u70b9\u8fdb\u884c\u9884\u5b98\u80fd\u56e2\u5316\uff08Scheme 1, path a\uff09[1]\u3002\u6beb\u65e0\u7591\u95ee\uff0c\u5bfb\u6c42\u4e00\u79cd\u50ac\u5316\u7684C(sp2)-H\u952e\u76f4\u63a5\u7fa7\u57fa\u5316\u7684\u65b9\u6cd5\uff08Scheme 1, path 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left\uff09[6]\u3002\u8fd9\u4e9b\u7ed3\u679c\u8ba9\u6709\u673a\u5316\u5b66\u5bb6\u4eec\u610f\u8bc6\u5230\uff0c\u65e0\u9700\u8d35\u91d1\u5c5e\u6216\u6709\u673a\u91d1\u5c5e\u8bd5\u5242\u8fdb\u884c\u7684\u50ac\u5316C(sp2)-H\u7fa7\u57fa\u5316\u7b56\u7565\u53ef\u80fd\u4f1a\u4e3aC(sp2)-H\u952e\u5b98\u80fd\u56e2\u5316\u4e0e\u7fa7\u57fa\u5316\u63d0\u4f9b\u65b0\u7684\u57fa\u7840\u77e5\u8bc6\u3002\u53d7\u6b64\u542f\u53d1\uff0c\u4f5c\u8005\u8bbe\u60f3\u662f\u5426\u53ef\u901a\u8fc7\u57fa\u4e8e\u4f4d\u7f6e\u9009\u62e9\u6027\u7684[1,4]-Ni\u8fc1\u79fb[7]\u7684\u4e32\u8054\u8fc7\u7a0b\u5b9e\u73b0CO2\u63d2\u5165\u8fdc\u7a0bC(sp2)-H\u952e\u7684\u53cd\u5e94\uff08Scheme 2\uff09\u3002\u4f5c\u8005\u5728\u5f00\u59cb\u7814\u7a76\u4e4b\u524d\uff0c\u8fd9\u79cd\u7b56\u7565\u80fd\u5426\u6210\u529f\u672a\u77e5\uff0c\u56e0\u4e3a\u6709\u4ee5\u4e0b\u4e24\u70b9\u539f\u56e0\uff1a\uff081\uff09\u76ee\u524d\uff0c\u5728\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u4e2d\u672a\u51fa\u73b0\u50ac\u5316\u7684[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u7684\u62a5\u9053\uff1b\uff082\uff09\u5728\u53cd\u5e94\u4e2d\u7531\u4e8eC(sp3)-Br\u952e\u4e0e\u7094\u57fa\u6d3b\u6cfc\u53cd\u5e94\u4f4d\u70b9\u7684\u5b58\u5728\uff0c\u4f1a\u9047\u5230\u4f4d\u7f6e\u9009\u62e9\u6027\u7684\u95ee\u9898[8]\u3002\u5982\u679c\u8be5\u8bbe\u60f3\u80fd\u591f\u6210\u529f\uff0c\u8fd9\u5c06\u6210\u4e3a\u8fd8\u539f\u6027\u4ea4\u53c9\u5076\u8054\u53cd\u5e94\u9886\u57df\u7684\u91cd\u5927\u7a81\u7834\uff0c\u53ef\u5b9e\u73b0\u5176\u4ed6\u65b9\u6cd5\u4e0d\u80fd\u5b9e\u73b0\u7684C(sp2)-H\u952e\u529f\u80fd\u5316\u7684\u53cd\u5e94\uff0c\u4ece\u800c\u4f5c\u4e3a\u4e00\u79cd\u65b0\u578b\u53cd\u5e94\u6a21\u5f0f\u3002 \u53cd\u5e94\u6761\u4ef6\u4f18\u5316 \u9996\u5148\uff0c\u4f5c\u8005\u4ee5\u5316\u5408\u72691a\u4f5c\u4e3a\u6a21\u677f\u5e95\u7269\u3001\u4ee5CO2\u4e3a\u7fa7\u57fa\u6e90\u5bf9\u53cd\u5e94\u6761\u4ef6\u8fdb\u884c\u7b5b\u9009\uff08Table 1\uff09\u3002\u4e0d\u51fa\u6240\u6599\uff0c\u5f53\u4f7f\u7528\u4ee5\u524d\u62a5\u9053\u7684\u82b3\u57fa\u5364\u5316\u7269\u4e0eCO2\u7684\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u53cd\u5e94\u6761\u4ef6\u65f6[9]\uff0c\u4ec5\u89c2\u5bdf\u5230\u5fae\u91cf\u7684\u76ee\u6807\u4ea7\u72692a\uff0c\u4e3b\u8981\u662f\u751f\u6210\u4e86CO2\u4e0e\u7094\u57fa\u53cd\u5e94\u7684\u526f\u4ea7\u72692a\u2019\u3002\u5728\u5bf9\u53cd\u5e94\u53c2\u6570\u8fdb\u884c\u4f18\u5316\u540e\uff0c\u53d1\u73b0NiBr2.diglyme\u3001L5\u4e0eMn89Cr11\u7684\u7ec4\u5408\u4f7f\u7528\u662f\u53cd\u5e94\u6210\u529f\u7684\u5173\u952e\uff0c\u80fd\u4ee577%\u7684\u4ea7\u7387\u4e0e\u4f18\u79c0\u7684\u4f4d\u7f6e\u9009\u62e9\u6027\uff082a:2a\u2019=94:6\uff09\u751f\u6210\u76ee\u6807\u4ea7\u72692a(Table 1, entry 1)\u3002\u968f\u540e\uff0c\u4f5c\u8005\u5bf9\u914d\u4f53\u6838\u5fc3\u9aa8\u67b62,2-\u8054\u5421\u5576\u7684\u7535\u6027\u6216\u4f4d\u963b\u8fdb\u884c\u8c03\u6574\uff0c\u53d1\u73b0\u5bf9\u53cd\u5e94\u6d3b\u6027\u6709\u4e0d\u53ef\u5ffd\u89c6\u7684\u5f71\u54cd\uff08Table 1, entries 2-5\uff09\uff1b\u663e\u8457\u5730\uff0c\u4f7f\u7528\u5176\u4ed6\u7c7b\u91d1\u5c5e\u8fd8\u539f\u5242\u66ff\u4ee3Mn89Cr11\u65f6\uff0c\u53cd\u5e94\u7684\u4ea7\u7387\u4e0e\u9009\u62e9\u6027\u5747\u660e\u663e\u964d\u4f4e\uff08Table1, entries 6-8\uff09\uff1b\u5c3d\u7ba1\u6709\u4eba\u8ba4\u4e3aCr\u539f\u5b50\u7684\u5b58\u5728\u53ef\u80fd\u51b3\u5b9a\u4e86\u53cd\u5e94\u7684\u4f4d\u7f6e\u9009\u62e9\u6027\uff0c\u800centry 7\u4e0eentry 8\u8bc1\u660e\u7ed3\u679c\u5374\u76f8\u53cd\uff0c\u76ee\u524d\u4f5c\u8005\u5bf9Cr\u7684\u4f5c\u7528\u4e5f\u65e0\u6cd5\u89e3\u91ca\u3002\u63a5\u7740\u4f5c\u8005\u53d1\u73b0\u4f7f\u7528Ni(cod)2\u4f5c\u4e3a\u50ac\u5316\u5242\u6216DMSO\u66ff\u6362DMF\u4f5c\u4e3a\u6eb6\u5242\u65f6\uff08entry 9 and entry 10\uff09\uff0c\u5747\u65e0\u6cd5\u8fbe\u5230\u7406\u60f3\u7684\u7ed3\u679c\u3002\u7136\u800c\uff0c\u5f53\u4f7f\u7528\u5bf9\u7a7a\u6c14\u4e0e\u6e7f\u6c14\u7a33\u5b9a\u7684NiBr2(L5)2\u4f5c\u4e3a\u50ac\u5316\u5242\u65f6\uff0c\u80fd\u4ee5\u4f18\u79c0\u7684\u4ea7\u7387\u4e0e\u4f4d\u7f6e\u9009\u62e9\u6027\u751f\u6210\u76ee\u6807\u4ea7\u7269\uff0c\u4f5c\u8005\u4ee5\u6b64\u4e3a\u6700\u4f18\u53cd\u5e94\u6761\u4ef6\uff08Table 1, entry 11\uff09\u3002 \u5e95\u7269\u62d3\u5c55 \u5728\u786e\u5b9a\u6700\u4f18\u53cd\u5e94\u6761\u4ef6\u540e\uff0c\u4f5c\u8005\u5bf9\u8be5\u53cd\u5e94\u7684\u5e95\u7269\u8303\u56f4\u8fdb\u884c\u63a2\u7d22\uff08Table 2\uff09\u3002\u4f5c\u8005\u53d1\u73b0\uff0c\u5e95\u7269\u7ed3\u6784\u4e2d\u542b\u6709\u786b\u919a(2d)\u3001\u7532\u6c27\u82b3\u70c3(2b)\u3001\u4e09\u6c1f\u7532\u57fa\u884d\u751f\u7269(2c and 2i)\u6216\u6742\u73af\uff082o\uff09\u65f6\uff0c\u53cd\u5e94\u5747\u80fd\u5b8c\u7f8e\u5730\u8fdb\u884c\u3002\u751a\u81f3\u82b3\u57fa\u5364\u5316\u7269\uff082g, 2h and 2r\uff09\u6216\u6709\u673a\u787c\u5316\u7269\uff082e\uff09\u4e5f\u80fd\u517c\u5bb9\u3002\u503c\u5f97\u6ce8\u610f\u7684\u662f\uff0c\u7094\u70c3\u90e8\u5206\u65e0\u8bba\u662f\u5927\u4f4d\u963b\u82b3\u57fa\uff082m\uff09\u6216\u8102\u80aa\u70f7\u57fa\u53d6\u4ee3\uff082j-l\uff09\u5e95\u7269\u4e5f\u80fd\u4ee5\u4f18\u79c0\u7684\u4ea7\u7387\u83b7\u5f97\u76ee\u6807\u4ea7\u7269\u3002\u65e0\u8bba\u662f\u7094\u70c3\u9aa8\u67b6\u4e0a\u7684\u4f4d\u963b\u56e0\u7d20\u8fd8\u662f\u60f0\u6027\u4e8c\u7ea7\u70f7\u57fa\u6eb4\u5316\u7269\uff082p and 2q\uff09\u5747\u80fd\u4ee5\u8f83\u9ad8\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807C(sp2)-H\u952e\u7fa7\u57fa\u5316\u4ea7\u7269\u3002\u6709\u8da3\u7684\u662f\uff0c\u82b3\u73af\u4e0a\u5b58\u5728\u4e0d\u540c\u53d6\u4ee3\u57fa\u65f6\u4e5f\u4e0d\u80fd\u963b\u6b62[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u7684\u53d1\u751f\uff0c\u5c3d\u7ba1\u53cd\u5e94\u7684\u4ea7\u7387\u6bd4\u8f83\u4f4e\uff082r and 2s\uff09\uff1b\u6b64\u5916\uff0c\u901a\u8fc7Si\u539f\u5b50\u94fe\u63a5\u70f7\u57fa\u6eb4\u5316\u7269\u5c24\u5176\u91cd\u8981\uff0c\u4e5f\u80fd\u83b7\u5f97\u76ee\u6807\u7fa7\u9178\u4ea7\u7269\uff082t-w\uff09\uff0c\u6240\u5f97\u7fa7\u9178\u4ea7\u7269\u53ef\u901a\u8fc7\u540e\u671f\u7684C-Si\u952e\u65ad\u88c2\u751f\u6210\u975e\u7a20\u73af\u7c7b\u5316\u5408\u7269\uff08Scheme 4, bottom\uff09\u3002 \u5316\u5408\u72692a-w\u7684\u6210\u529f\u5408\u6210\uff0c\u4f5c\u8005\u8ba4\u4e3a\u7b80\u5355\u70ef\u57fa\u5364\u5316\u7269\u4f5c\u4e3a\u5e95\u7269\u65f6\u5e94\u8be5\u4e5f\u80fd\u53d1\u751f\u7c7b\u4f3c\u7684[1,4]-Ni\u8fc1\u79fb\u7684\u8fdc\u7a0bC(sp2)-H\u952e\u7fa7\u57fa\u5316\u53cd\u5e94\u3002\u5982Scheme 3\u6240\u793a\uff0c\u4f5c\u8005\u5c06\u53cd\u5e94\u6eb6\u5242\u7531DMF\u6539\u4e3aDMA\u540e\uff0c\u5176\u4ed6\u6761\u4ef6\u4e0d\u53d8\uff0c\u53d1\u73b0\u65e0\u8bba\u662f\u70f7\u57fa\u53d6\u4ee3\u8fd8\u662f\u82b3\u57fa\u53d6\u4ee3\u7684\u70ef\u57fa\u6eb4\u5316\u7269\u5747\u80fd\u53d1\u751f\u76ee\u6807C(sp2)-H\u952e\u76f4\u63a5\u7fa7\u57fa\u5316\u751f\u6210\u76ee\u6807\u4ea7\u72694a\uff08E\/Z=2.4\/1\uff09\u4e0e4b(E\/Z=3.3\/1), \u5c3d\u7ba1\u5e95\u72693a\u4e0e3b\u5747\u4e3aE\/Z\u5f02\u6784\u4f53\u6df7\u5408\u7269\u3002\u5b9e\u9a8c\u7ed3\u679c\u8868\u660e\uff0c\u5e95\u7269\u4e0e\u50ac\u5316Ni(0)\u7269\u79cd\u53d1\u751f\u6c27\u5316\u52a0\u6210\u5f62\u6210\u7684Ni(II)\u7269\u79cd\u5728\u53d1\u751f[1,4]-Ni\u8fc1\u79fb\u6b65\u9aa4\u4e4b\u524d\u4f1a\u53d1\u751fE\/Z\u5f02\u6784\u5316\uff0c\u8fc7\u7a0b\u4e2d\u53ef\u80fd\u5b58\u5728\u5361\u5bbe\u7c7b\u4e2d\u95f4\u4f53[10]\u3002 \u884d\u751f\u5316\u7814\u7a76 \u6b64\u5916\uff0c\u4f5c\u8005\u4e3a\u4e86\u8bc1\u660e[1,4]-Ni\u8fc1\u79fb\u6280\u672f\u7684\u5e94\u7528\u4ef7\u503c\uff0c\u5bf9\u7fa7\u57fa\u5316\u4ea7\u7269\u8fdb\u884c\u4e86\u4e00\u7cfb\u5217\u7684\u884d\u751f\u5316\u5e94\u7528\uff08Scheme 4\uff09\u3002\u7fa7\u91782a\u62162b\u5728\u4e24\u79cd\u4e0d\u540c\u7684\u53cd\u5e94\u6761\u4ef6\u4e0b\u80fd\u591f\u5408\u6210\u5f02\u8272\u6ee1\u916e\u6216\u82ef\u915e\u7c7b\u590d\u6742\u5206\u5b50\uff0c\u7fa7\u91782a\u5728TFA( 10mol%)\u3001NBS\u5b58\u5728\u6761\u4ef6\u4e0b\u53d1\u751f\u6eb4\u5185\u916f\u5316\u4ee583%\u7684\u4ea7\u7387\u751f\u6210\u82ef\u915e\u7c7b\u5316\u5408\u72695\uff0c\u800c\u5728H2SO4\u4f5c\u7528\u6761\u4ef6\u4e0b\u80fd\u4ee588%\u7684\u4ea7\u7387\u751f\u6210\u82ef\u915e\u7c7b\u5316\u5408\u72696\uff1b\u76f8\u4f3c\u5730\uff0c2a\u5728PdCl(MeCN)2\u50ac\u5316\u4f5c\u7528\u4e0b\u80fd\u4ee588%\u7684\u4ea7\u7387\u83b7\u5f97\u5f02\u8272\u6ee1\u916e\u7c7b\u5316\u5408\u72697\uff0c\u540c\u65f62b\u5728H2SO4\u5b58\u5728\u6761\u4ef6\u4e0b\u80fd\u4ee562%\u7684\u4ea7\u7387\u83b7\u5f97\u5f02\u8272\u6ee1\u916e\u7c7b\u4f3c\u72698(dr 4.2:1)\u3002\u91cd\u8981\u7684\u662f\uff0c\u5b58\u5728Si\u539f\u5b50\u7684\u7fa7\u91782w \u5728TMSCHN2\u3001H2O2\u4f5c\u7528\u4e0b\u80fd\u591f\u53d1\u751fC-Si\u952e\u65ad\u88c2\u4ee543%\u7684\u4ea7\u7387\u83b7\u5f97\u591a\u7f9f\u57fa\u7fa7\u9178\u916f\u7c7b\u5316\u5408\u72699\uff0c\u8fdb\u4e00\u6b65\u8bc1\u5b9e\u4e86\u8be5\u7fa7\u57fa\u5316\u53cd\u5e94\u65b9\u6cd5\u7684\u5b9e\u7528\u6027\u3002 \u53cd\u5e94\u673a\u7406\u63a2\u7d22 \u6700\u540e\uff0c\u4f5c\u8005\u5bf9\u53cd\u5e94\u673a\u7406\u8fdb\u884c\u4e86\u521d\u6b65\u7814\u7a76(Scheme 5)\u3002\u9996\u5148\uff0c\u4f5c\u8005\u4ee53c\u4f5c\u4e3a\u5e95\u7269\u8fdb\u884c\u4e86\u540c\u4f4d\u7d20\u6807\u8bb0\u7814\u7a76(Scheme 5, top)\uff0c3c\u5728\u6700\u4f73\u53cd\u5e94\u6761\u4ef6\u4e0b\u8fdb\u884c\u53cd\u5e94\u4ee545%\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807\u4ea7\u72694c\uff0c\u5176\u4e2d4c\u7684\u70ef\u57fa\u4f4d\u7684\u6c18\u4ee3\u7387\u5927\u4e8e95%\uff0c\u8bc1\u660e\u5728CO2\u63d2\u5165\u76ee\u6807C(sp2)-H\u952e\u524d\u5728\u70ef\u57fa\u90bb\u4f4dC(sp2)-H\u952e\u4e0a\u53d1\u751f\u4e86[1,4]-Ni\u8fc1\u79fb\uff1b\u6709\u8da3\u7684\u662f\uff0c\u5bf9\u5316\u5408\u72693d\u8fdb\u884c\u8fd8\u539f\u6027\u7fa7\u57fa\u5316\u53cd\u5e94\u65f6\uff0c\u53d1\u73b0\u4e86\u660e\u663e\u7684\u5206\u5b50\u5185\u52a8\u529b\u5b66\u540c\u4f4d\u7d20\u6548\u5e94\uff08KH\/KD=5:1; Scheme 5, top right\uff09\uff0c\u4f5c\u8005\u901a\u8fc73a\u4e0e3c\u7684\u53cd\u5e94\u901f\u7387\u5bf9\u6bd4\u672a\u53d1\u73b0\u5206\u5b50\u95f4\u52a8\u529b\u5b66\u540c\u4f4d\u7d20\u6548\u5e94\u3002\u8fd9\u4e9b\u7ed3\u679c\u8868\u660e\uff0c\u5728\u53d1\u751f[1,4]-Ni\u8fc1\u79fb\u524d\u6216\u8fc1\u79fb\u540e\u5b58\u5728\u4e00\u4e2a\u51b3\u901f\u6b65\u9aa4\u3002\u5c3d\u7ba1\u5982\u6b64\uff0c\u4ecd\u4e0d\u77e5CO2\u63d2\u5165\u4e0e[1,4]-Ni\u8fc1\u79fb\u8fc7\u7a0b\u662f\u53d1\u751f\u5728Ni(I)\u8fd8\u662fNi(II)\u91d1\u5c5e\u4e2d\u5fc3\u4e0a\u3002\u56e0\u800c\uff0c\u4f5c\u8005\u5c06\u6ce8\u610f\u529b\u8f6c\u79fb\u5230\u6c27\u5316\u52a0\u6210\u5f62\u6210\u7684\u70ef\u57fa\u6216\u82b3\u57fa\u954d\u91d1\u5c5e\u914d\u5408\u7269\u4e2d\u95f4\u7684\u5206\u79bb\u4e0a\uff08Scheme 5, bottom\uff09\u3002\u6709\u8da3\u7684\u662f\uff0c\u82b3\u57fa\uff08\u70ef\u57fa\uff09\u5364\u5316\u7269\u4e0eNi(cod)2\u548cTMEDA\u6216L2\u5728THF\u6eb6\u5242\u4e2d\u80fd\u53d1\u751f\u53cd\u5e94\u5206\u522b\u751f\u6210\u954d\u6709\u673a\u91d1\u5c5e\u7edc\u5408\u726910\u4e0e11\u3002\u4f5c\u8005\u4ee5\u8fd9\u4e24\u79cd\u954d\u7edc\u5408\u7269\u4f5c\u4e3a\u53cd\u5e94\u7269\u8fdb\u884c\u7fa7\u57fa\u5316\u53cd\u5e94\u7814\u7a76\uff0c\u53d1\u73b010\u4ec5\u5728L5\u5b58\u5728\u6761\u4ef6\u4e0b\u5c31\u80fd\u4e0eCO2\u53d1\u751f\u53cd\u5e94\u4ee549%\u7684\u4ea7\u7387\u751f\u6210\u76ee\u6807\u7fa7\u57fa\u5316\u4ea7\u72694a, \u8bc1\u5b9e2,2\u2019-\u8054\u5421\u5576\u914d\u4f53\u5bf9\u53d1\u751f\u76ee\u6807\u7fa7\u57fa\u5316\u53cd\u5e94\u7684\u91cd\u8981\u6027\uff1b\u66f4\u91cd\u8981\u7684\u662f\uff0c10\u4e0e11\u5747\u80fd\u5728\u65e0\u5916\u52a0\u91d1\u5c5e\u8fd8\u539f\u5242\u5b58\u5728\u6761\u4ef6\u4e0b\u53d1\u751f\u7fa7\u57fa\u5316\u53cd\u5e94\u751f\u6210\u76ee\u6807\u4ea7\u72694a, 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