{"id":233640,"date":"2022-03-06T06:00:24","date_gmt":"2022-03-05T22:00:24","guid":{"rendered":"\/\/m.iemloyee.com\/?p=233640"},"modified":"2022-03-05T21:00:40","modified_gmt":"2022-03-05T13:00:40","slug":"%e5%a4%a9%e5%a4%a7%e6%9d%9c%e5%b8%8c%e6%96%87%e7%ad%89-adv-sci-%ef%bc%9amoo2x%e8%a1%a8%e9%9d%a2%e4%bb%b7%e6%80%81%e6%95%88%e5%ba%94%e5%af%b9nrr%e7%9a%84%e5%bd%b1%e5%93%8d","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=233640","title":{"rendered":"\u5929\u5927\u675c\u5e0c\u6587\u7b49 Adv. Sci.\uff1aMoO2+x\u8868\u9762\u4ef7\u6001\u6548\u5e94\u5bf9NRR\u7684\u5f71\u54cd"},"content":{"rendered":"

\u3010\u80cc\u666f\u4ecb\u7ecd\u3011<\/strong><\/p>\n

\u6c28\u6c14\uff08ammonia, NH3<\/sub>\uff09\u662f\u4e00\u79cd\u91cd\u8981\u7684\u5546\u54c1\u539f\u6599\uff0c\u5e7f\u6cdb\u7528\u4e8e\u751f\u4ea7\u80a5\u6599\u548c\u5851\u6599\u7b49\u4ea7\u54c1\u3002\u5176\u4e2d\uff0c\u5229\u7528\u53ef\u518d\u751f\u7535\u529b\uff0c\u7535\u5316\u5b66\u6c2e\u8fd8\u539f\u53cd\u5e94\uff08nitrogen reduction reaction, NRR\uff09\u53ef\u5728\u73af\u5883\u538b\u529b\u548c\u6e29\u5ea6\u4e0b\u8fdb\u884c\uff0c\u663e\u8457\u964d\u4f4e\u80fd\u8017\u548cCO2<\/sub>\u6392\u653e\uff0c\u662fHaber-Bosch\u6cd5\u7684\u4e00\u79cd\u6709\u5438\u5f15\u529b\u7684\u66ff\u4ee3\u65b9\u6cd5\u3002\u7136\u800c\uff0c\u76ee\u524d\u7f3a\u4e4f\u80fd\u591f\u8bf1\u5bfcN2<\/sub>\u5206\u5b50\u5f3a\u70c8\u5438\u9644\u548c\u6709\u6548\u6d3b\u5316\u7684\u50ac\u5316\u5242\uff0c\u9650\u5236\u4e86NH3<\/sub>\u7684\u751f\u6210\u901f\u7387\u3002\u540c\u65f6\uff0c\u7531\u4e8e\u8d28\u5b50\u6613\u4e8e\u6d3b\u5316\uff0c\u66f4\u5bb9\u6613\u53d1\u751f\u7ade\u4e89\u6027\u6790\u6c22\u53cd\u5e94\uff08HER\uff09\uff0c\u4ece\u800c\u5bfc\u81f4\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FE\uff09\u964d\u4f4e\u3002<\/p>\n

\u7531\u4e8eFeMo\u8f85\u52a9\u56e0\u5b50\u5728\u6c34\u73af\u5883\u4e2d\u7684\u9ad8\u6548\u548c\u9009\u62e9\u6027\u6c28\u8f6c\u5316\u80fd\u529b\uff0c\u4e00\u76f4\u662fNRR\u50ac\u5316\u5242\u7684\u542f\u53d1\u6765\u6e90\u3002\u5728N2<\/sub>\u8f6c\u5316\u4e3aNH3<\/sub>\u7684\u8fc7\u7a0b\u4e2d\uff0cMo\u4e2d\u5fc3\u5728Mo(III)\u548cMo(VI)\u4e4b\u95f4\u5faa\u73af\uff0c\u5176\u4e2dMo\u8c03\u6574\u5176\u4ef7\u6001\u7684\u80fd\u529b\u5bf9\u4e8e\u5b8c\u6210\u8fdc\u7aef\u9014\u5f84\u6dfb\u52a06\u4e2a\u7535\u5b50\u548c6\u4e2a\u8d28\u5b50\u4ee5\u4ea7\u751fNH3<\/sub>\u81f3\u5173\u91cd\u8981\u3002\u4f46\u662f\uff0cMo\u5728\u78b1\u6027\u6c34\u7535\u89e3\u8d28\u4e2d\u7684\u70ed\u529b\u5b66\u7a33\u5b9a\u5f62\u5f0f\u662fMoO4<\/sub>2-<\/sup>\uff0c\u662f\u4e00\u79cd\u4e0d\u9002\u5408\u591a\u76f8\u50ac\u5316\u7684\u53ef\u6eb6\u79bb\u5b50\u3002\u5728Mo\u91d1\u5c5e\u8150\u8680\u4e2d\uff0cMo\u7684\u56fa\u4f53\u6c27\u5316\u5f62\u5f0f\uff0c\u4e3b\u8981\u662f\u5728\u78b1\u6027\u6761\u4ef6\u4e0b\u7684Mo(IV)O2<\/sub>\uff0c\u540c\u65f6\u5b58\u5728Mo(IV)O(OH)2<\/sub>\u548cMo(VI)O3<\/sub>\uff0c\u5076\u5c14\u4f1a\u5f62\u6210\u949d\u6001\u5c42\u4ee5\u9632\u6b62MoO4<\/sub>2-<\/sup>\u7684\u6eb6\u89e3\u3002\u56e0\u6b64\uff0c\u5728\u78b1\u6027\u7535\u89e3\u8d28\u4e2d\u5f62\u6210\u81ea\u9650\u6027\u6c27\u5316\u5c42\uff0c\u5c31\u6709\u53ef\u80fd\u7814\u7a76\u4e0d\u540c\u4ef7\u6001\u7684Mo\u4f5c\u4e3a\u591a\u76f8\u50ac\u5316\u5242\u3002
\n \"\"<\/p>\n

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

\u8fd1\u65e5\uff0c\u5929\u6d25\u5927\u5b66\u675c\u5e0c\u6587\u6559\u6388\u3001\u5fb7\u514b\u8428\u65af\u5dde\u5927\u5b66\u5965\u65af\u6c40\u5206\u6821Yuanyue Liu\u548c\u829d\u52a0\u54e5\u5927\u5b66Chong Liu\uff08\u5171\u540c\u901a\u8baf\u4f5c\u8005\uff09\u7b49\u4eba<\/strong>\u62a5\u9053\u4e86\u4e00\u79cd\u5bcc\u542b\u8868\u9762Mo6+<\/sup>\u7684MoO2+x<\/sub>\u50ac\u5316\u5242\u3002\u4f5c\u8005\u5229\u7528\u6c34\u70ed\u6cd5\u5408\u6210\u4e86MoO2+x<\/sub>\uff0c\u5176\u4e2dMo(VI)O4<\/sub>2-<\/sup>\u7684\u76f4\u63a5\u8fd8\u539f\u4f7fMoO2<\/sub>\u5bcc\u542b\u8868\u9762Mo6+<\/sup>\uff08MoO2+x<\/sub>\uff09\u3002X\u5c04\u7ebf\u5149\u7535\u5b50\u80fd\u8c31\uff08XPS\uff09\u3001\u5f00\u8def\u7535\u538b\uff08OCV\uff09\u548c\u7535\u8377\u8f6c\u79fb\u7535\u963b\u6d4b\u91cf\u5747\u663e\u793a\u8868\u9762\u5b58\u5728Mo6+<\/sup>\uff0c\u800c\u5085\u91cc\u53f6\u53d8\u6362\u7ea2\u5916\u5149\u8c31\uff08FT-IR\uff09\u8868\u5f81\u786e\u5b9a\u4e86Mo6+<\/sup>\u7684\u5b58\u5728\u5f62\u5f0f\u4e3a(MoO3<\/sub>)n<\/sub>\u7c07\u3002MoO2<\/sub>\u4e0a\u7684\u8868\u9762Mo6+<\/sup>\u5728pH=13\u6eb6\u6db2\u4e2d\u7a33\u5b9a\uff0c\u800c\u5bf9\u7167\u7ec4Mo(VI)O3<\/sub>\u7acb\u5373\u6eb6\u89e3\u3002\u8fd9\u4e9b\u8868\u9762Mo6+<\/sup>\u53ef\u4ee5\u5728\u9ad8\u6d53\u5ea6KOH\u6eb6\u6db2\uff085 M\uff09\u4e2d\u88ab\u8680\u523b\u6389\u4ee5\u5f62\u6210MoO2<\/sub>\uff0c\u4ece\u800c\u80fd\u591f\u7814\u7a76Mo\u5bf9NRR\u7684\u4ef7\u6001\u6548\u5e94\u3002\u5728\u64cd\u4f5c\u7535\u538b\u4e0b\uff0cMo6+<\/sup>\u548cMo4+<\/sup>\u5747\u663e\u793a\u8fd8\u539f\u4e3aMo3+<\/sup>\u3002\u5f53\u7528\u4f5cNRR\u50ac\u5316\u5242\u65f6\uff0c\u6240\u5236\u5907\u7684MoO2+x<\/sub>\u663e\u793a\u51fa3.95 \u00b5g mgcat.<\/sub>-1<\/sup> h-1<\/sup>\u7684\u9ad8NH3<\/sub>\u4ea7\u7387\u3002\u5728-0.2 V vs. RHE\u65f6\u5177\u670922.1%\u7684\u9ad8\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FE\uff09\uff0c\u8fdc\u4f18\u4e8e\u5bf9\u7167\u7ec4MoO2<\/sub>\u50ac\u5316\u5242\u76841.06 \u00b5g mgcat.<\/sub>-1<\/sup> h-1<\/sup>\u4ea7\u7387\u548c9.4% FE\uff0c\u8868\u660e\u663e\u8457\u7684NRR\u6d3b\u6027\u6e90\u4e8e\u8868\u9762\u7684\u9ad8\u4ef7Mo6+<\/sup>\u3002\u5728\u6ca1\u6709\u8868\u9762Mo6+<\/sup>\u4e0b\uff0c\u8d28\u5b50\u53ef\u4ee5\u5f88\u5bb9\u6613\u5730\u8f6c\u79fb\u5230MoO2<\/sub>\u8868\u9762\uff0c\u5e76\u4e14HER\u6d3b\u6027\u663e\u8457\u63d0\u9ad8\u3002\u56e0\u6b64\uff0c\u8868\u9762Mo6+<\/sup>\u6291\u5236\u4e86HER\uff0c\u4fc3\u8fdb\u4e86\u6c2e\u5438\u9644\u3002\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\u8868\u660e\uff0c\u8868\u9762\u9644\u7740\u7684(MoO3<\/sub>)3<\/sub>\u7c07\u964d\u4f4e\u4e86\u7b2c\u4e00\u4e2a\u52a0\u6c22\u6b65\u9aa4\u7684\u6d3b\u5316\u80fd\u5792\u3002\u7814\u7a76\u6210\u679c\u4ee5\u9898\u4e3a\u201cSurface Valence State Effect of MoO2+x<\/sub> on Electrochemical Nitrogen Reduction\u201d<\/strong>\u53d1\u5e03\u5728\u56fd\u9645\u8457\u540d\u671f\u520aAdv. Sci.<\/strong><\/em>\u4e0a\u3002<\/p>\n

\u3010\u56fe\u6587\u89e3\u8bfb\u3011<\/strong><\/p>\n

\u56fe\u4e00\u3001MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684\u5f62\u8c8c\u8868\u5f81 \u00a9 2022 The Authors<\/span><\/strong>
\n \"\"\uff08a-b\uff09NRR\u548cHER\u5728\u539f\u59cbMoO2<\/sub>\u548c\u5bcc\u542b\u8868\u9762Mo6+<\/sup>\u7684MoO2+x<\/sub>\u4e0a\u7684\u793a\u610f\u56fe\uff1b<\/p>\n

\uff08c\uff09MoO2+x<\/sub>\/CC\u7684SEM\u56fe\u50cf\uff0c\u63d2\u56fe\u662f\u653e\u5927\u7684SEM\u56fe\u50cf\uff1b<\/p>\n

\uff08d\uff09MoO2+x<\/sub>\u7684TEM\u56fe\u50cf\uff0c\u63d2\u56fe\u662fSAED\u56fe\u6848\uff1b<\/p>\n

\uff08e\uff09MoO2+x<\/sub>\u7684HAADF-STEM\u56fe\u50cf\uff1b<\/p>\n

\uff08f\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684XRD\u56fe\u8c31\u3002<\/p>\n

\u56fe\u4e8c\u3001MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684\u7ed3\u6784\u8868\u5f81\u00a0\u00a9 2022 The Authors<\/span><\/strong>
\n \"\"\uff08a\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684Mo 3d XPS\u5149\u8c31\uff1b<\/p>\n

\uff08b\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684O 1s XPS\u5149\u8c31\uff1b<\/p>\n

\uff08c\uff09Ar\u79bb\u5b50\u6df1\u5ea6\u8680\u523b\u7684\u793a\u610f\u56fe\uff1b<\/p>\n

\uff08d\uff09\u5728Ar\u79bb\u5b50\u6df1\u5ea6\u8680\u523b\u4e00\u7cfb\u5217\u65f6\u95f4\u540e\uff0c\u8bb0\u5f55\u7684MoO2+x<\/sub>\u7684Mo 3d XPS\u5149\u8c31\uff1b<\/p>\n

\uff08e\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684\u5f00\u8def\u7535\u538b\uff08OCV\uff09\u884c\u4e3a\uff1b<\/p>\n

\uff08f\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u5728OCV\u4e0b\u7684\u7535\u5316\u5b66\u963b\u6297\u8c31\uff08EIS\uff09\u66f2\u7ebf\u3002<\/p>\n

\u56fe\u4e09\u3001MoO2+x<\/sub>\u7684NRR\u7535\u5316\u5b66\u6027\u80fd\u00a0\u00a9 2022 The Authors<\/span><\/strong>
\n \"\"\uff08a\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u5728N2<\/sub>\u9971\u548c\u4e0eAr\u9971\u548c\u76840.1 M KOH\u7535\u89e3\u8d28\u4e2d\u7684LSV\u66f2\u7ebf\uff1b<\/p>\n

\uff08b\uff09\u4f7f\u7528MoO2+x<\/sub>\u4f5c\u4e3a\u50ac\u5316\u5242\uff0c\u5728\u7535\u538b\u4e3a-0.2 V vs. RHE\u4e0b\uff0c\u975b\u915a\u6307\u793a\u5242\u67d3\u8272\u7684\u7535\u89e3\u8d28\u5728\u4e0d\u540c\u65f6\u95f4\u6bb5\u7684UV-vis\u5149\u8c31\uff1b<\/p>\n

\uff08c\uff09MoO2+x<\/sub>\u5728-0.1\u5230-0.5 V vs. RHE\u7684\u5916\u52a0\u7535\u4f4d\u4e0b\uff0c\u8fde\u7eed\u6c28\u4ea7\u91cf\u968f\u65f6\u95f4\u7684\u53d8\u5316\uff1b<\/p>\n

\uff08d\uff09\u5728\u6bcf\u4e2a\u7ed9\u5b9a\u7535\u4f4d\u4e0bMoO2+x<\/sub>\u548cMoO2<\/sub>\u7684NH3<\/sub>\u4ea7\u7387\u548cFE\uff1b<\/p>\n

\uff08e\uff09MoO2+x<\/sub>\u5728-0.2 V vs. RHE\u4e0b\u7684\u5faa\u73af\u7a33\u5b9a\u6027\uff1b<\/p>\n

\uff08f\uff09\u5bf9\u7167\u5b9e\u9a8c\u8868\uff0c\u6240\u7814\u7a76\u50ac\u5316\u5242\u4e0a\u7684NH3<\/sub>\u4ea7\u91cf\u3002<\/p>\n

\u56fe\u56db\u3001\u540c\u4f4d\u7d20N\u6807\u8bb0\u5b9e\u9a8c\u6d4b\u5b9a\u6027\u80fd\u00a0\u00a9 2022 The Authors<\/span><\/strong>
\n \"\"\uff08a, e\uff09\u4ee5\u9a6c\u6765\u9178\u4e3a\u5185\u6807\u7269\uff0c\u6d4b\u5b9a\u4e0d\u540c\u6d53\u5ea614<\/sup>NH4<\/sub>+<\/sup>\u7684\u6807\u51c614<\/sup>NH4<\/sub>Cl\u548c\u4e0d\u540c\u6d53\u5ea615<\/sup>NH4<\/sub>+<\/sup>\u768415<\/sup>NH4<\/sub>Cl\u76841<\/sup>H NMR\u8c31\uff1b<\/p>\n

\uff08b, f\uff09\u5728\u53cd\u5e94\u6301\u7eed\u65f6\u95f4\u4e3a1 h\u548c3 h\u7684NRR\u8bd5\u9a8c\u540e\uff0c\u5728-0.2 V vs. RHE\u4e0b\u52a0\u516514<\/sup>N2<\/sub>\u548c15<\/sup>N2<\/sub>\uff0cNRR\u6d4b\u8bd5\u540e\u7535\u89e3\u8d28\u76841<\/sup>H NMR\u5149\u8c31\uff1b<\/p>\n

\uff08c, g\uff09\u6807\u51c614<\/sup>NH4<\/sub>Cl\u548c15<\/sup>NH4<\/sub>Cl\u4e0e\u5cf0\u9762\u79ef\u6bd4\u7684\u5bf9\u5e94\u6807\u51c6\u66f2\u7ebf\uff1b<\/p>\n

\uff08d, h\uff09\u5728-0.2 V vs. RHE\u4e0b\u53cd\u5e94\u6301\u7eed1\u548c3 h\u540e\uff0c\u5f53\u52a0\u516514<\/sup>N2<\/sub>\u548c15<\/sup>N2<\/sub>\u65f6MoO2+x<\/sub>\u7684\u6c28\u4ea7\u7387\u3002<\/p>\n

\u56fe\u4e94\u3001\u7406\u8bba\u6a21\u62df\u8ba1\u7b97\u00a0\u00a9 2022 The Authors<\/span><\/strong>
\n \"\"\uff08a-b\uff09MoO2+x<\/sub>\u548cMoO2<\/sub>\u7684\u539f\u5b50\u6a21\u578b\uff0cN2<\/sub>\u5206\u5b50\u88ab\u5438\u9644\uff0c\u7528\u4e8eDFT\u6a21\u62df\uff1b<\/p>\n

\uff08c-d\uff09\u8ba1\u7b97\u4e86\u6cbf\u4ea4\u66ff\u8def\u5f84\u548c\u8fdc\u7aef\u8def\u5f84\u7684MoO2+x<\/sub>\u548cMoO2<\/sub>\u4e0aNRR\u7684Gibbs\u81ea\u7531\u80fd\u3002<\/p>\n

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

\u7efc\u4e0a\u6240\u8ff0\uff0c\u4f5c\u8005\u5236\u5907\u4e86\u5bcc\u542b\u8868\u9762Mo6+<\/sup>\u7684MoO2+x<\/sub>\uff0c\u5176NH3<\/sub>\u4ea7\u7387\u9ad8\u8fbe3.95 \u00b5g mgcat.<\/sub>-1<\/sup> h-1<\/sup>\uff0c\u5e76\u4e14\u5728-0.2 V vs. RHE\u65f6\u5177\u670922.1%\u7684\u9ad8\u6cd5\u62c9\u7b2c\u6548\u7387\uff08FE\uff09\u3002\u901a\u8fc7\u5b9e\u9a8c\u8868\u5f81\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\u90fd\u8868\u660e\uff0c\u663e\u7740\u589e\u5f3a\u7684NRR\u6d3b\u6027\u6e90\u81ea\u4e8e\u8868\u9762\u4e0a\u7684\u9ad8\u4ef7Mo6+<\/sup>\u3002\u6b64\u5916\uff0c\u8fd8\u8fdb\u884c\u4e86\u5404\u79cd\u5bf9\u7167\u5b9e\u9a8c\u548c\u5b9a\u91cf\u540c\u4f4d\u7d20\u6807\u8bb0\u5b9e\u9a8c\uff0c\u4ee5\u786e\u4fdd\u7535\u5316\u5b66\u6c2e\u8fd8\u539f\u5b9e\u9a8c\u7ed3\u679c\u7684\u51c6\u786e\u6027\u3002\u8be5\u5de5\u4f5c\u8868\u660e\uff0c\u6784\u5efa\u72ec\u7279\u7684\u4ef7\u6001\u662f\u8bbe\u8ba1\u7528\u4e8e\u6c2e\u8fd8\u539f\u4ea7\u7387NH3<\/sub>-timeion\u7684\u4f18\u826f\u7535\u50ac\u5316\u5242\u7684\u6709\u6548\u65b9\u6cd5\u3002<\/p>\n

\u6587\u732e\u94fe\u63a5\uff1aSurface Valence State Effect of MoO2+x<\/sub> on Electrochemical Nitrogen Reduction<\/a><\/strong>. Adv. Sci.<\/em>, 2022<\/strong>, DOI: 10.1002\/advs.202104857.<\/p>\n

\u672c\u6587\u7531CQR\u7f16\u8bd1\u3002<\/p>\n

\u6b22\u8fce\u5927\u5bb6\u5230\u6750\u6599\u4eba\u5ba3\u4f20\u79d1\u6280\u6210\u679c\u5e76\u5bf9\u6587\u732e\u8fdb\u884c\u6df1\u5165\u89e3\u8bfb\uff0c\u6295\u7a3f\u90ae\u7bb1\uff1atougao@cailiaoren.com.<\/p>\n

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