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\u2462 \u901a\u8fc7AIMD\u8ba1\u7b97\u63ed\u793a\u4e86Co\u7f3a\u9677\u7684\u5f15\u5165\u53ef\u4ee5\u6709\u6548\u6d3b\u5316Co3<\/sub>O4<\/sub>\u4e2d\u7684\u516b\u9762\u4f53\u4f4d\u70b9\uff0c\u52a0\u901fH2<\/sub>O\u7684\u52a8\u529b\u5b66\u5438\u9644\u901f\u7387\u3002\u540c\u65f6\u53ef\u4ee5\u4fc3\u8fdbOER\u4e2d\u4ea7\u7269O2<\/sub>\u5206\u5b50\u7684\u89e3\u79bb\u3002<\/section>\n
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\u2463 In suit ATR-SEIRAS\u8868\u5f81\u8fdb\u4e00\u6b65\u8bc1\u5b9e\u4e86AIMD\u8ba1\u7b97\u7ed3\u679c\uff0c\u6b64\u5916\u8fdb\u4e00\u6b65\u8bc1\u660e\u4e86Co\u7f3a\u9677\u53ef\u4ee5\u4fc3\u8fdbOH*\u8131\u8d28\u5b50\u8fc7\u7a0b\u5f62\u6210OOH*\u3002\u800cex suit XPS\u5219\u8bc1\u660e\u4e86Co\u7f3a\u9677\u53ef\u4ee5\u4fc3\u8fdbCo3<\/sub>O4<\/sub>\u8868\u9762\u5728OER\u8fc7\u7a0b\u4e2d\u7684\u8868\u9762\u91cd\u6784\u8fc7\u7a0b\u548cOH*\u7684\u8131\u6c22\u8fc7\u7a0b\u3002<\/section>\n
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\u00a0\u00a0<\/section>\n<\/section>\n<\/section>\n<\/section>\n<\/section>\n<\/section>\n
\u56fe\u6587\u89e3\u6790<\/strong><\/section>\n
\"1\"Figure 1. (a) The simulation results of metal defect formation energy with metal monomers and metal chlorides as products and oxygen defect formation energy of Mn3<\/sub>O4<\/sub>, Fe2<\/sub>O3<\/sub>, Fe3<\/sub>O4<\/sub>, Co3<\/sub>O4<\/sub>, and NiO, respectively. (b) Schematic diagram of metal defects etched out by chlorine plasma. (c) DFT-predicted and XPS characterization for determination of metal defect concentrations in Mn3<\/sub>O4<\/sub>, Fe2<\/sub>O3<\/sub>, Co3<\/sub>O4<\/sub>\u00a0and NiO.<\/section>\n
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DFT\u8ba1\u7b97\u53d1\u73b0\u901a\u8fc7\u5c06\u91d1\u5c5e\u7f3a\u9677\u5236\u5907\u8fc7\u7a0b\u4e2d\u7684\u4ea7\u7269\u7531\u91d1\u5c5e\u539f\u5b50\u8f6c\u53d8\u4e3a\u91d1\u5c5e\u6c2f\u5316\u7269\u53ef\u4ee5\u5927\u5e45\u964d\u4f4e\u91d1\u5c5e\u7f3a\u9677\u7684\u5f62\u6210\u80fd\u751a\u81f3\u4f4e\u4e8e\u6c27\u7f3a\u9677\u3002\u57fa\u4e8eDFT\u9884\u6d4b\uff0c\u5728\u6c2f\u6c14\u7b49\u79bb\u5b50\u4f53\u534f\u52a9\u4e0b\uff0c\u5728Mn3<\/sub>O4<\/sub>\uff0cFe2<\/sub>O3<\/sub>\uff0cCo3<\/sub>O4<\/sub>\uff0cNiO\u8868\u9762\u6210\u529f\u5f15\u5165\u91d1\u5c5e\u7f3a\u9677\uff0c\u4e14\u91d1\u5c5e\u7f3a\u9677\u6d53\u5ea6\u4e0eDFT\u8ba1\u7b97\u4e2d\u5f62\u6210\u7684\u8d8b\u52bf\u51e0\u4e4e\u4e00\u81f4\u3002\u66f4\u91cd\u8981\u7684\u662f\uff0c\u901a\u8fc7\u7b80\u5355\u8c03\u8282\u7b49\u79bb\u5b50\u4f53\u7684\u5904\u7406\u65f6\u95f4\u5373\u53ef\u5b9e\u73b0\u91d1\u5c5e\u7f3a\u9677\u6d53\u5ea6\u7684\u8c03\u63a7\u3002<\/section>\n
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\"2\"Figure 2. Deconvoluted (a) Co 2p and (b) O 1s spectra of Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3, Co3<\/sub>O4<\/sub>-CP-6. (c) Co K-edge XANES spectra of Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3, Co3<\/sub>O4<\/sub>-CP-6 (Insets magnify the region of 7700.7-7709.4 eV). (d) 2D Charge density difference distribution (between catalyst with and without one Co vacancy in the Co3<\/sub>O4<\/sub>\u00a0cell) by DFT calculation. (e) Rietveld refinement results of Co3<\/sub>O4<\/sub>-CP-3. (f) Co K-edge EXAFS of Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3, Co3<\/sub>O4<\/sub>-CP-6, shown in R-space. Data are k3<\/sup>\u00a0weighted and not phase-corrected.<\/section>\n
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XPS\u3001EXAFS\u3001XRD\u7cbe\u4fee\u7ed3\u679c\u8868\u660e\uff0c\u7531\u4e8e\u91d1\u5c5e\u7f3a\u9677\u5f62\u6210\u88ab\u663e\u8457\u964d\u4f4e\u81f3\u4f4e\u4e8e\u6c27\u7f3a\u9677\uff0c\u8be5\u6cd5\u53ef\u4ee5\u5728\u51e0\u4e4e\u907f\u514d\u751f\u6210\u6c27\u7f3a\u9677\u7684\u57fa\u7840\u4e0a\u5f15\u5165\u4e30\u5bcc\u7684\u91d1\u5c5e\u7f3a\u9677\u3002\u6b64\u5916\uff0c\u7535\u8377\u5bc6\u5ea6\u5dee\u5206\u8ba1\u7b97\u8868\u660e\uff0cCo\u7f3a\u9677\u7684\u5f15\u5165\u8bf1\u53d1\u4e86Co\u539f\u5b50\u5468\u56f4\u7684\u7535\u5b50\u79bb\u57df\uff0c\u4ece\u800c\u4f7fCo\u5448\u73b0\u66f4\u9ad8\u7684\u4ef7\u6001\uff0c\u8fd9\u4e5f\u4e0eXPS\u548cXANES\u4e2d\u7684\u7ed3\u679c\u76f8\u4e00\u81f4\u3002\u6b64\u5916\uff0cCo\u7a7a\u4f4d\u51fa\u73b0\u7684\u5927\u91cf\u79bb\u57df\u7535\u5b50<\/span>\u53ef\u4ee5\u5145\u5f53\u7535\u5316\u5b66\u8fc7\u7a0b\u4e2d\u7684\u8f7d\u6d41\u5b50\u4ece\u800c\u964d\u4f4eCo3<\/sub>O4<\/sub>\u5728\u7535\u5316\u5b66\u8fc7\u7a0b\u4e2d\u7684\u963b\u6297\u3002<\/section>\n
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\"3\"Figure 3. (a, d) HRTEM image of Co3<\/sub>O4<\/sub>-CP-3. (b) Polarization curves of OER on Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3 and Co3<\/sub>O4<\/sub>-CP-6 in 1 M KOH recorded at 5 mV s\u20131<\/sup>\u00a0(forward scan). (c) Tafel plots of Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3 and Co3<\/sub>O4<\/sub>-CP-6. (e) Electrochemical impedance spectroscopy of Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3 and Co3<\/sub>O4<\/sub>-CP-6 at 1.58 V vs. RHE. (f) Chronoamperometry response curves at a constant potential of 1.53 V.<\/section>\n
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TEM\u56fe\u7247\u8868\u9762Co\u7f3a\u9677\u7684\u5f15\u5165\u5728Co3<\/sub>O4<\/sub>\u8868\u9762\u5f62\u6210\u4e86\u4e00\u5c42\u65e0\u5b9a\u578b\u533a\u57df\uff0c\u4e14\u968f\u7740\u5904\u7406\u65f6\u95f4\u5ef6\u957f\uff0c\u65e0\u5b9a\u578b\u533a\u57df\u9010\u6e10\u53d8\u539a\u3002OER\u6d3b\u6027\u6d4b\u8bd5<\/span>\u8868\u660e\uff0c\u5728\u5f15\u5165\u91d1\u5c5e\u7f3a\u9677\u540e\u5927\u5e45\u964d\u4f4e\u4e86\u50ac\u5316\u5242\u7684\u8fc7\u7535\u52bf\u3001\u5854\u83f2\u5c14\u659c\u7387\u3001\u7535\u8377\u8f6c\u79fb\u963b\u6297\uff0c\u4e14\u572840000 s\u7684\u7a33\u5b9a\u6027\u6d4b\u8bd5\u4e2d\uff0c\u7535\u6d41\u5bc6\u5ea6\u672a\u89c1\u660e\u663e\u4e0b\u964d\u3002<\/section>\n
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\"4\"Figure 4. Radial distribution function (RDF) for octahedral Co of (a) Co3<\/sub>O4<\/sub>-C and (b) Co3<\/sub>O4<\/sub>-CP-3 during 0-1200 fs by AIMD. Results of integration of RDF for octahedral Co of (c) Co3<\/sub>O4<\/sub>-C and (d) Co3<\/sub>O4<\/sub>-CP-3 at 3000 fs by AIMD. Calculated free energy diagram for OER of octahedral and tetrahedral Co in (e, f) Co3<\/sub>O4<\/sub>-C, (g, h) Co3<\/sub>O4<\/sub>-CP-3, (i, j) Co3<\/sub>O4<\/sub>-CP-6 at zero potential and the theoretical overpotential.<\/section>\n
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AIMD\u8ba1\u7b97\u8868\u660e\uff0cCo\u7f3a\u9677\u7684\u5f15\u5165\u53ef\u4ee5\u5927\u5e45\u6d3b\u5316Co3<\/sub>O4<\/sub>\u4e2d\u7684\u516b\u9762\u4f53\u4f4d\u70b9\uff0c\u4f7f\u5176\u5728\u66f4\u77ed\u65f6\u95f4\u5185\u5438\u9644\u66f4\u591a\u7684\u6c34\u5206\u5b50\u3002\u6b64\u5916Co\u7f3a\u9677\u8fd8\u53ef\u4ee5\u4fc3\u8fdbOER\u4ea7\u7269O2<\/sub>\u5206\u5b50\u7684\u89e3\u79bb\u3002\u800cDFT\u8ba1\u7b97\u5219\u8bf4\u660e\u9002\u5b9c\u6d53\u5ea6\u7684\u91d1\u5c5e\u7f3a\u9677\u53ef\u4ee5\u663e\u8457\u964d\u4f4eCo3<\/sub>O4<\/sub>\u56db\u9762\u4f53\u548c\u516b\u9762\u4f53\u6d3b\u6027\u4f4d\u4e0a\u7684OER\u7406\u8bba\u8fc7\u7535\u52bf\u3002<\/section>\n
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\"8\"Figure 5. (a) Deconvoluted Co 2p spectra Co3<\/sub>O4<\/sub>-CP-3 were carried out the applied potential. (b) Comparison of overall Co 2p spectra of Co3<\/sub>O4<\/sub>-CP-3 were carried out the applied potential. (c) Comparison of the Co3+<\/sup>\/Co2+<\/sup>\u00a0ratio and cyclic voltammetry spectra of Co3<\/sub>O4<\/sub>-C and Co3<\/sub>O4<\/sub>-CP-3 at different potentials. (d) In situ ATR-SEIRAS of (d) Co3<\/sub>O4<\/sub>-C and (e) Co3<\/sub>O4<\/sub>-CP-3 recorded during the multi-potential steps<\/section>\n
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Ex suit XPS\u8868\u660eOER\u4e2dCo3O4\u4e2dCo\u7684\u4ef7\u6001\u4e0d\u65ad\u4e0a\u5347\uff0c\u7136\u800c\u5728Co\u7f3a\u9677\u5bfc\u81f4\u4e86Co\u4ef7\u6001\u7684\u8d77\u59cb\u4e0a\u5347\u7535\u4f4d\u7684\u63d0\u524d\u548c\u7ec8\u6001Co3+\/2+<\/sup>\u6bd4\u503c\u7684\u5347\u9ad8\u3002\u800c\u4e14Co\u4ef7\u6001\u7684\u8d77\u59cb\u4e0a\u5347\u7535\u4f4d\u4e0eCV\u66f2\u7ebf\u4e2d\uff0c\u6c27\u5316\u5cf0\u7684\u4f4d\u7f6e\u51e0\u4e4e\u5b8c\u5168\u543b\u5408\u3002\u8fd9\u8bf4\u660eCo\u7f3a\u9677\u4fc3\u8fdb\u4e86Co3<\/sub>O4<\/sub>\u8868\u9762\u7684\u91cd\u6784\u548cOH*\u7684\u8131\u8d28\u5b50\u8fc7\u7a0b\u3002In suit ATR-SEIRAS\u5219\u76f4\u63a5\u8bc1\u660e\u4e86\u5728\u5f15\u5165Co\u7f3a\u9677\u540e\uff0cCo3<\/sub>O4<\/sub>\u53ef\u4ee5\u5728\u66f4\u4f4e\u7535\u4f4d\u5438\u9644\u66f4\u591a\u7684\u6c34\u5206\u5b50\uff0c\u5373,\u5927\u5927\u52a0\u901f\u4e86H2<\/sub>O\u7684\u5438\u9644\u52a8\u529b\u5b66\u8fc7\u7a0b\u3002\u6b64\u5916\uff0cOOH*\u4e5f\u5728\u66f4\u4f4e\u7535\u4f4d\u88ab\u89c2\u5bdf\u5230\uff0c\u8bf4\u660e\u4e86Co\u7f3a\u9677\u5bf9OH*\u2192O*\u8fd9\u4e00\u8fc7\u7a0b\u7684\u4fc3\u8fdb\u4f5c\u7528\uff0c\u540c\u65f6\uff0c\u8fd8\u901a\u8fc7\u4fc3\u8fdb\u6c27\u6c14\u5206\u5b50\u7684\u91ca\u653e\u8fc7\u7a0b\u6709\u6548\u6291\u5236\u4e86OOH*\u5728\u9ad8\u7535\u4f4d\u7684\u7d2f\u8ba1\uff0c\u4ece\u800c\u907f\u514d\u4e86\u4ea7\u7269\u96be\u4ee5\u89e3\u79bb\u5360\u636e\u6d3b\u6027\u4f4d\u70b9\u7684\u95ee\u9898\u3002\u4e0a\u8ff0\u5b9e\u9a8c\u7ed3\u679c\u4e0e\u524d\u6587\u7684AIMD\u548cDFT\u8ba1\u7b97\u7ed3\u679c\u9ad8\u5ea6\u4e00\u76f4\u5730\u8bc1\u660e\u4e86Co\u7f3a\u9677\u5bf9OER\u8fc7\u7a0b\u7684\u52a8\u529b\u5b66\u548c\u70ed\u529b\u5b66\u4fc3\u8fdb\u4f5c\u7528\u3002<\/section>\n
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\"9\"\u200bFigure 6. (a) Polarization curves of ORR on Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3 and Co3<\/sub>O4<\/sub>-CP-6 in 0.1 M KOH recorded at 1600 rpm rotating speed (5 mV s\u20131<\/sup>). (b) The electron transfer number n and peroxide () yields with respect to the total oxygen reduction products. (c) schematic diagram describes the fabrication of zinc-air battery. (d) A LED light display screen powered by two home-made Zn\u2013air batteries in series with Co3<\/sub>O4<\/sub>-CP-3 as the air-cathode. (e) Charging and discharging polarization curves for the Zn\u2013air battery using Co3<\/sub>O4<\/sub>-C, Co3<\/sub>O4<\/sub>-CP-3 and Co3<\/sub>O4<\/sub>-CP-6 cathodes.\u00a0 (f) Long term galvanostatic charge discharge curve of zinc-air batteries with Co3<\/sub>O4<\/sub>-C and Co3<\/sub>O4<\/sub>-CP-3 based air cathode with 5 min charging and 5 min discharging at a current density 1 mA cm\u2212<\/sup>2<\/sup>.<\/section>\n
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\u9664\u63d0\u5347OER\u6d3b\u6027\u4e4b\u5916\uff0cCo\u7f3a\u9677\u540c\u6837\u589e\u5f3a\u4e86\u50ac\u5316\u5242\u7684ORR\u6d3b\u6027\u3002\u5728\u5c06\u5176\u7ec4\u88c5\u6210Zn-Air\u7535\u6c60\u540e\uff0c\u5c55\u73b0\u51fa\u4e86\u66f4\u4f4e\u7684\u5145\u7535\u7535\u538b\u548c\u653e\u7535\u7535\u538b\u3002\u5e76\u4e14\u5728\u957f\u8fbe600 h\u7684\u7a33\u5b9a\u6027\u6d4b\u8bd5\u4e2d\uff0c\u4fdd\u6301\u7a33\u5b9a\u3002<\/section>\n
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\u603b\u7ed3\u4e0e\u5c55\u671b<\/strong><\/section>\n
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