{"id":14076,"date":"2018-08-02T00:00:01","date_gmt":"2018-08-01T16:00:01","guid":{"rendered":"https:\/newsletter.sinica.edu.tw\/?p=14076"},"modified":"2021-08-12T15:09:19","modified_gmt":"2021-08-12T07:09:19","slug":"%e8%a7%a3%e6%9e%90%e9%87%91%e5%b1%ac%e9%85%b5%e7%b4%a0%e5%82%ac%e5%8c%96%e6%a9%9f%e5%88%b6%e7%82%ba%e8%a8%ad%e8%a8%88%e4%ba%ba%e9%80%a0%e8%a7%b8%e5%aa%92%e7%94%a8%e6%96%bc%e8%83%bd%e6%ba%90%e8%bd%89","status":"publish","type":"post","link":"https:\/newsletter.sinica.edu.tw\/14076\/","title":{"rendered":"\u3010\u5c08\u6b04\u3011\u89e3\u6790\u91d1\u5c6c\u9175\u7d20\u50ac\u5316\u6a5f\u5236\u70ba\u8a2d\u8a08\u4eba\u9020\u89f8\u5a92\u7528\u65bc\u80fd\u6e90\u8f49\u63db\u7684\u95dc\u9375"},"content":{"rendered":"

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\n\u5716\u4e00 \u9435\u9435\u6c2b\u5316\u9175\u7d20\u53ca\u5176\u6d3b\u5316\u4e2d\u5fc3<\/p>\n

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\u5728\u6c2b\u6c23\u4ee3\u8b1d\u904e\u7a0b\u4e2d\uff0c\u6c2b\u6c23\u9996\u5148\u9375\u7d50\u5230\u9435\u50ac\u5316\u4e2d\u5fc3\u4e0a\uff0c\u900f\u904e\u96d9\u786b\u57fa\u4e0a\u7684\u80fa\u57fa\uff0c\u5c07\u6c2b\u6c23\u9032\u884c\u7570\u76f8\u5206\u89e3\u6210\u8cea\u5b50\u548c\u91d1\u5c6c\u6c2b\u5316\u7269\u3002\u8cea\u5b50\u85c9\u7531\u80fa\u57fa\u7684\u5354\u52a9\uff0c\u50b3\u905e\u9060\u96e2\u96d9\u9435\u4e2d\u5fc3\uff0c\u9435\u6c2b\u5316\u7269\u4e5f\u6703\u8f49\u8b8a\u70ba\u9084\u539f\u614b\u9435\u6838\u53ca\u8cea\u5b50\uff0c\u5f8c\u8005\u5c07\u85c9\u7531\u80fa\u57fa\u50b3\u51fa\u9435\u4e2d\u5fc3\uff1b\u540c\u6642\uff0c\u9435\u6838\u518d\u88ab\u6c27\u5316\u56de\u5230\u8d77\u59cb\u614b\uff0c\u7b49\u5f85\u4e0b\u4e00\u6b21\u7684\u4ee3\u8b1d\u53cd\u61c9\u3002\u5728\u6587\u737b\u4e2d\uff0c\u6240\u6709\u5be6\u9a57\u5ba4\u4e2d\u5408\u6210\u7684\u76f8\u4f3c\u5316\u5408\u7269\uff0c\u4e26\u4e0d\u5177\u6709\u9435\u6c2b\u5316\u5408\u7269\u8f49\u8b8a\u70ba\u9084\u539f\u614b\u9435\u6838\u53ca\u8cea\u5b50\u7684\u80fd\u529b\u3002\u7531\u65bc\u9435\u6c2b\u5316\u5408\u7269\u70ba\u71b1\u529b\u5b78\u4e0a\u6700\u7a69\u5b9a\u7684\u7269\u7a2e\uff0c\u8981\u5c07\u5176\u8f49\u8b8a\u6210\u8cea\u5b50\u4e26\u975e\u81ea\u767c\u6027\u53cd\u61c9\u3002[5]\u5728\u6211\u5011\u7684\u7814\u7a76\u4e2d\uff0c\u5339\u914d\u96d9\u9435\u6838\u5fc3\u53ca\u8cea\u5b50\u53d7\u9ad4\u7684pKa\u503c\u70ba\u6c7a\u5b9a\u6027\u7684\u95dc\u9375\u3002[6] \u7d93\u7531\u9069\u7576\u8abf\u63a7\u96d9\u9435\u4e2d\u5fc3\u8def\u6613\u58eb\u9178\u9e7c\u5ea6\uff0c\u6211\u5011\u53ef\u4ee5\u6210\u529f\u5730\u5f15\u5c0e\u8cea\u5b50\u8f49\u79fb\u5230\u8cea\u5b50\u53d7\u9ad4\u4e0a\u6216\u96d9\u9435\u6838\u5fc3\u4e0a\u3002\u9019\u7a2e\u53ef\u9006\u53cd\u61c9\u662f\u9996\u6b21\u5728\u6587\u737b\u4e0a\u5831\u5c0e\u7684\uff0c\u9019\u7d50\u679c\u5c0d\u65bc\u8a2d\u8a08\u5206\u5b50\u89f8\u5a92\u7528\u65bc\u71c3\u6599\u96fb\u6c60\u7684\u967d\u6975\u6750\u6599\u6709\u5f88\u5927\u7684\u5e6b\u52a9\u3002<\/p>\n

\u548c\u5927\u591a\u6578\u7531\u9175\u7d20\u5354\u52a9\u7684\u50ac\u5316\u53cd\u61c9\u4e00\u6a23\uff0c\u8abf\u63a7\u8cea\u5b50\u548c\u96fb\u5b50\u8f49\u79fb\u662f\u9019\u985e\u50ac\u5316\u6700\u91cd\u8981\u7684\u95dc\u9375\uff0c\u4f8b\u5982\uff0c\u5728Tyrosinase\u50ac\u5316\u9130\u82ef\u4e8c\u915a\uff08benzene-1,2-diol\uff09\u70ba1,2-\u82ef\u918c\uff081,2-benzoquinone\uff09\u7684\u904e\u7a0b\u4e2d\uff0cTyrosinase\u4e2d\u7684\u916a\u6c28\u9178\u5b98\u80fd\u57fa\u5354\u52a9\u524d\u8005\u812b\u53bb\u5169\u500b\u8cea\u5b50\u53ca\u5169\u500b\u96fb\u5b50\u3002[7] \u4e00\u822c\u800c\u8a00\uff0c\u7576\u8cea\u5b50\u5316\u5148\u767c\u751f\u5728\u50ac\u5316\u4e2d\u5fc3\u4e0a\uff0c\u5176\u9084\u539f\u96fb\u4f4d\u5c31\u88ab\u5927\u5e45\u964d\u4f4e\uff0c\u6216\u7576\u50ac\u5316\u4e2d\u5fc3\u5148\u884c\u63a5\u53d7\u96fb\u5b50\uff0c\u9084\u539f\u614b\u7684\u50ac\u5316\u4e2d\u5fc3\u5c0d\u8cea\u5b50\u7684\u89aa\u548c\u529b\u5c31\u88ab\u52a0\u5f37\uff1b[8] \u7136\u800c\uff0c\u6b32\u4f7f\u8cea\u5b50\u5316\u6216\u9084\u539f\u53cd\u61c9\u5148\u767c\u751f\uff0c\u4e3b\u8981\u727d\u6d89\u5230\u50ac\u5316\u6838\u5fc3\u4e2d\u03c3\u96fb\u5b50\u5c0d\u5f37\u5ea6\u3001\u8def\u6613\u58eb\u9178\u9e7c\u5ea6\uff0c\u4ee5\u53ca\u6700\u4f4e\u672a\u586b\u6eff\u5206\u5b50\u8ecc\u57df\uff08lowest unoccupied molecular orbital, LUMO\uff09\u7684\u80fd\u968e\u3002\u56e0\u6b64\u8cea\u5b50\u5316\u548c\u9084\u539f\u614b\u53cd\u61c9\u4f3c\u4e4e\u5177\u6709\u76f8\u4e92\u5f71\u97ff\u7684\u56e0\u679c\u95dc\u4fc2\uff0c\u4f46\u4e0d\u76e1\u7136\u3002\u5728\u67d0\u4e9b\u7279\u6b8a\u7684\u689d\u4ef6\u4e0b\uff0c\u8cea\u5b50\u548c\u96fb\u5b50\u8f49\u79fb\u53ef\u540c\u6642\u767c\u751f\u3002[9] \u5728\u9019\u985e\u8cea\u5b50-\u96fb\u5b50\u5076\u5408\u53cd\u61c9\u4e2d\uff0c\u8cea\u5b50\u5316\u53ca\u9084\u539f\u614b\u7684\u4e2d\u9593\u7269\u6c92\u6709\u751f\u6210\uff0c\u53cd\u61c9\u76f4\u63a5\u7565\u904e\u6b64\u5169\u7a2e\u9ad8\u80fd\u968e\u6b65\u9a5f\uff0c\u9054\u5230\u6700\u7d42\u7522\u7269\u3002\u5728\u6700\u8fd1\u7684\u7814\u7a76\u4e2d\uff0c\u6211\u5011\u627e\u5230\u4e00\u7cfb\u7d71\u53ef\u9032\u884c\u6b64\u985e\u53cd\u61c9\u3002[10] \u85c9\u7531\u8cea\u5b50-\u96fb\u5b50\u5076\u5408\u53cd\u61c9\uff0c\u6211\u5011\u8b49\u660e\u50ac\u5316\u53cd\u61c9\u6240\u9700\u7684\u80fd\u8017\u4ee5\u53ca\u904e\u96fb\u4f4d\u5927\u5e45\u964d\u4f4e\uff0c\u53d6\u800c\u4ee3\u4e4b\uff0c\u53cd\u61c9\u901f\u5ea6\u548c\u50ac\u5316\u6548\u7387\u986f\u8457\u589e\u52a0\uff08\u5716\u4e8c\u5de6\uff09\u3002\u4e5f\u5c31\u662f\u8aaa\uff0c\u8cea\u5b50-\u96fb\u5b50\u5076\u5408\u53cd\u61c9\u540c\u6642\u63d0\u4f9b\u71b1\u529b\u5b78\u53ca\u52d5\u529b\u5b78\u4e0a\u7684\u76ca\u8655\u3002<\/p>\n

\u9175\u7d20\u5728\u7d93\u7531\u6578\u5104\u5e74\u7684\u6f14\u5316\u904e\u7a0b\u5f8c\uff0c\u767c\u5c55\u51fa\u9ad8\u50ac\u5316\u6548\u7387\u3001\u9ad8\u9078\u64c7\u6027\u53ca\u4f4e\u80fd\u8017\u7684\u7cfb\u7d71\u3002\u900f\u904e\u5f88\u591a\u7684\u7814\u7a76\u62bd\u7d72\u525d\u7e6d\u4e0b\uff0c\u9175\u7d20\u7684\u9019\u4e9b\u512a\u9ede\u53ca\u5176\u8abf\u63a7\u7684\u56e0\u5b50\uff0c\u9010\u6f38\u88ab\u767c\u6398\u51fa\u4f86\u3002\u89e3\u958b\u9019\u4e9b\u79d8\u5bc6\uff0c\u53ea\u662f\u4e00\u500b\u958b\u7aef\uff0c\u7dca\u63a5\u8457\u543e\u7b49\u53ef\u628a\u9019\u4e9b\u77e5\u8b58\u904b\u7528\u5728\u8a2d\u8a08\u4eba\u9020\u89f8\u5a92\u4e0a\uff08\u5716\u4e8c\u53f3\uff09\uff0c[11] \u5efa\u7acb\u4e00\u500b\u6c38\u7e8c\u7684\u7d93\u6fdf\u3002<\/p>\n

\"\"
\n\u5716\u4e8c\uff08\u5de6\uff09\u900f\u904e\u8cea\u5b50-\u96fb\u5b50\u5206\u6b21\u53cd\u61c9\u53ca\u8cea\u5b50-\u96fb\u5b50\u5076\u5408\u53cd\u61c9\u4f86\u7522\u6c2b\u7684\u793a\u610f\u5716\u3002\uff08\u53f3\uff09\u8a2d\u8a08\u542b\u4eba\u9020\u89f8\u5a92\u4e4b\u96fb\u6975\u6750\u6599\u7528\u65bc\u8cea\u5b50\/\u6c2b\u6c23\u4ee3\u8b1d\u53cd\u61c9\u3002<\/p>\n

\u53c3\u8003\u6587\u737b
\n[1] Lubitz, W.; Ogata, H.; R\u00fcdiger, O.; Reijerse, E. Hydrogenases. Chem. Rev. 2014, 114, 4081\u20134148.
\n[2] Liu, Y.-C.; Yen, T.-H.; Tseng, Y.-J.; Hu, C.-H.; Lee, G.-H.; Chiang, M.-H. Electron Delocalization from the Fullerene Attachment to the Diiron Core within the Active-Site Mimics of [FeFe]Hydrogenase. Inorg. Chem. 2012, 51, 5997\u20135999.
\n[3] Chu, K.-T.; Liu, Y.-C.; Huang, Y.-L.; Lee, G.-H.; Tseng, M.-C.; Chiang, M.-H. Redox Communication within Multinuclear Iron-Sulfur Complexes Related to Electronic Interplay in the Active Site of [FeFe]Hydrogenase. Chem. Eur. J. 2015, 21, 6852\u20136861.
\n[4] Yen, T.-H.; He, Z.-C.; Lee, G.-H.; Tseng, M.-C.; Shen, Y.-H.; Tseng, T.-W.; Liaw, W.-F.; Chiang, M.-H. Reduced Thione Ligation is Preferred over Neutral Phosphine Ligation in Diiron Biomimics Regarding Electronic Functionality: a Spectroscopic and Computational Investigation. Chem. Commun. 2017, 53, 332\u2013335.
\n[5] Liu, Y.-C.; Chu, K.-T.; Jhang, R.-L.; Lee, G.-H.; Chiang, M.-H. [FeFe] Hydrogenase Active Site Modeling: a Key Intermediate Bearing a Thiolate Proton and Fe Hydride. Chem. Commun. 2013, 49, 4743\u20134749. (featured as a cover paper)
\n[6] Chu, K.-T.; Liu, Y.-C.; Huang, Y.-L.; Hsu, C.-H.; Lee, G.-H.; Chiang, M.-H. A Reversible Proton Relay Process Mediated by H-bonding Interaction in [FeFe]hydrogenase Modeling. Chem. Eur. J. 2015, 21, 10978\u201310982. (featured as a cover paper)
\n[7] Song, N.; Gagliardi, C. J.; Binstead, R. A.; Zhang, M. T.; Thorp, H.; Meyer, T. J. Role of Proton-Coupled Electron Transfer in the Redox Interconversion between Benzoquinone and Hydroquinone. J. Am. Chem. Soc. 2012, 134, 18538\u201318541.
\n[8] Liu, Y.-C.; Chu, K.-T.; Huang, Y.-L.; Hsu, C.-H.; Lee, G.-H.; Tseng, M.-C.; Chiang, M.-H. Protonation\/Reduction of Carbonyl-Rich Diiron Complexes and the Direct Observation of Triprotonated Species: Insights into the Electrocatalytic Mechanism of Hydrogen Formation. ACS Catal. 2016, 6, 2559\u20132576.
\n[9] Warren, J. J.; Tronic, T. A.; Mayer, J. M. Thermochemistry of Proton-coupled Electron Transfer Reagents and Its Implications. Chem. Rev. 2010, 110, 6961\u20137001.
\n[10] Chu, K.-T.; Liu, Y.-C.; Chung, M.-W.; Poerwoprajitno, A. R.; Lee, G.-H.; Chiang, M.-H. Energy-Efficient Hydrogen Evolution by FeS Electrocatalysts: Mechanistic Investigations. Inorg. Chem. 2018, 57, 7620\u20137630.
\n[11] Chung, M.-W.; Liu, Y.-C.; Yen, T.-H.; Chiang, M.-H. Bilayer Vesicles as a Noncovalent Immobilization Platform of Electrocatalysts for Energy Conversion in Neutral Aqueous Media. ChemElectroChem 2018, 5, 20\u201324. (featured as a cover paper)<\/p>\n","protected":false},"excerpt":{"rendered":"

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