{"id":256344,"date":"2023-12-05T06:18:09","date_gmt":"2023-12-04T22:18:09","guid":{"rendered":"\/\/m.iemloyee.com\/?p=256344"},"modified":"2023-12-04T19:24:07","modified_gmt":"2023-12-04T11:24:07","slug":"kaust%e5%bc%a0%e5%8d%8e%e5%bd%ac%e8%af%be%e9%a2%98%e7%bb%84angew-chem-%e9%87%91%e5%b1%9e%ef%bc%88%e7%be%9f%e5%9f%ba%ef%bc%89%e6%b0%a2%e6%b0%a7%e5%8c%96%e7%89%a9%e7%bb%93%e6%9e%84%e6%97%a0%e5%ba%8f","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=256344","title":{"rendered":"KAUST\u5f20\u534e\u5f6c\u8bfe\u9898\u7ec4Angew. Chem.: \u91d1\u5c5e\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u7ed3\u6784\u65e0\u5e8f\u4e0e\u7535\u50ac\u5316\u6790\u6c27\u6d3b\u6027\u7684\u5173\u8054"},"content":{"rendered":"

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

\u5f00\u53d1\u9ad8\u6548\u7684\u6790\u6c27\u53cd\u5e94\uff08OER\uff09\u7535\u50ac\u5316\u5242\u5e76\u4e86\u89e3\u5176\u7ed3\u6784-\u6027\u80fd\u5173\u7cfb\u5bf9\u80fd\u6e90\u8f6c\u6362\u548c\u50a8\u5b58\u81f3\u5173\u91cd\u8981\u3002\u7136\u800c\uff0c\u591a\u76f8\u7535\u50ac\u5316\u5242\u7684\u7ed3\u6784\u590d\u6742\u6027\u4f7f\u5f97\u9610\u660e\u5176\u52a8\u6001\u7ed3\u6784\u6f14\u53d8\u548c\u6790\u6c27\u53cd\u5e94\u673a\u5236\u4ea7\u751f\u4e86\u5de8\u5927\u7684\u6311\u6218\u3002\u57fa\u4e8e\u6b64\uff0c\u963f\u535c\u675c\u62c9\u56fd\u738b\u79d1\u6280\u5927\u5b66\u5f20\u534e\u5f6c\u6559\u6388\u548c\u97e9\u5b87\u6559\u6388\u5229\u7528\u8fc7\u6e21\u91d1\u5c5e\u6c27\u5316\u7269\uff0c\u786b\u5316\u7269\u548c\u7852\u5316\u7269\u4f5c\u4e3a\u6a21\u578b\u9884\u50ac\u5316\u5242\uff0c\u901a\u8fc7OER\u8fc7\u7a0b\u4e2d\u7684\u7ed3\u6784\u81ea\u91cd\u6784\u8fc7\u7a0b\uff0c\u5229\u7528\u53cd\u5e94\u524d\u786b\u5316\u7269\/\u7852\u5316\u7269\u9884\u50ac\u5316\u5242\u4e0e\u53cd\u5e94\u540e\u7684\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u4e4b\u95f4\u7684\u91d1\u5c5e-\u975e\u91d1\u5c5e\u952e\u957f\u5dee\u5f02\uff0c\u884d\u751f\u51fa\u4e0d\u540c\u7a0b\u5ea6\u7684\u7ed3\u6784\u65e0\u5e8f\u7684\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u3002\u7ed3\u679c\u8868\u660e\uff0c\u5177\u7528\u66f4\u9ad8\u7ed3\u6784\u65e0\u5e8f\u5ea6\u7684\u50ac\u5316\u5242\u663e\u793a\u51fa\u66f4\u4f18\u5f02\u7684\u6790\u6c27\u53cd\u5e94\u7535\u50ac\u5316\u6d3b\u6027\u3002\u539f\u4f4dX\u5c04\u7ebf\u5438\u6536\u7cbe\u7ec6\u7ed3\u6784\uff08XAFS\uff09\u5b9e\u9a8c\u63ed\u793a\u4e86\u6a21\u578b\u50ac\u5316\u5242\u5728OER\u8fc7\u7a0b\u4e2d\u7684\u7ed3\u6784\u65e0\u5e8f\u5ea6\u7684\u6f14\u53d8\u8fc7\u7a0b\u3002\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\u8868\u660e\uff0c\u7ed3\u6784\u65e0\u5e8f\u548c\u5c40\u57df\u7ed3\u6784\u7578\u53d8\u80fd\u591f\u8c03\u63a7\u50ac\u5316\u5242\u7535\u5b50\u7ed3\u6784\u548c\u8c03\u63a7\u50ac\u5316\u5242\u7684\u53cd\u5e94\u70ed\u52a8\u529b\u5b66\uff0c\u589e\u5f3a\u5176OER\u6027\u80fd\u3002\u672c\u5de5\u4f5c\u8bc1\u5b9e\u4e86OER\u7535\u50ac\u5316\u4e2d\u50ac\u5316\u5242\u7ed3\u6784\u65e0\u5e8f\u4e0e\u5176\u50ac\u5316\u6d3b\u6027\u4e4b\u95f4\u7684\u76f8\u5173\u6027\uff0c\u6709\u671b\u4e3a\u76f8\u5173\u50ac\u5316\u5242\u7684\u5236\u5907\u4ee5\u53ca\u63ed\u793a\u5176\u7ed3\u6784-\u6027\u80fd\u5173\u7cfb\u63d0\u4f9b\u65b0\u7684\u601d\u8def\u3002<\/p>\n

\"\"<\/p>\n

\u00a0<\/strong>\u4e09\u3001\u3010\u6838\u5fc3\u521b\u65b0\u70b9\u3011<\/strong><\/p>\n

1.\u672c\u5de5\u4f5c\u63d0\u51fa\u5229\u7528XAFS\u6765\u7814\u7a76\u50ac\u5316\u5242\u5728OER\u53cd\u5e94\u8fc7\u7a0b\u4e2d\u7ed3\u6784\u65e0\u5e8f\u6027\u7684\u53d8\u5316\u3002\u5e76\u7528Debye-Waller\u56e0\u5b50\u5bf9\u7ed3\u6784\u7684\u65e0\u5e8f\u5ea6\u8fdb\u884c\u5b9a\u91cf\u5206\u6790\u3002<\/p>\n

2.\u5c06\u7ed3\u6784\u65e0\u5e8f\u4e0e\u5176\u50ac\u5316\u672c\u5f81\u6d3b\u6027\u4e4b\u95f4\u8fdb\u884c\u5173\u8054\uff0c\u63ed\u793a\u4e86\u7ed3\u6784\u65e0\u5e8f\u4e0e\u50ac\u5316\u5242\u672c\u5f81\u6d3b\u6027\u4e4b\u95f4\u7684\u5173\u7cfb\uff0c\u6709\u671b\u4e3a\u76f8\u5173\u50ac\u5316\u5242\u7684\u5236\u5907\u63d0\u4f9b\u6307\u5bfc\u610f\u4e49\u3002<\/p>\n

\u00a0<\/strong>\u56db\u3001\u3010\u6570\u636e\u6982\u89c8\u3011<\/strong><\/p>\n

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\u00a0Figure 1<\/strong>. Characterizations of catalysts. a) HRTEM images of as-prepared Fe-Ni-OOH, Fe-Ni-O, Fe-Ni-S and Fe-Ni-Se. b) Fourier transformed magnitudes of Ni K<\/em>-edge EXAFS spectra for different pre-catalysts and in situ-derived catalysts. c) Bond length extracted from EXAFS fitting results for catalysts. d) Experimental Ni K<\/em>-edge XANES spectra for D-Fe-Ni-OOH, D(O)-Fe-Ni-OOH, D(S)-Fe-Ni-OOH and D(Se)-Fe-Ni-OOH. e) A schematic illustration showing the structural evolution from pre-catalysts to in situ-derived catalysts. Atoms with transparent color denote the corresponding dissolved anions during the reaction.<\/p>\n

\u7814\u7a76\u56e2\u961f\u5bf9\u6a21\u578b\u9884\u50ac\u5316\u5242\u6c27\u5316\u7269\u3001\u786b\u5316\u7269\u3001\u7852\u5316\u7269\u8fdb\u884c\u7ed3\u6784\u8868\u5f81\uff0cXAFS\u8868\u5f81\u7ed3\u679c\u8868\u660e\u884d\u751f\u7684\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269D(S)-Fe-Ni-OOH, D(Se)-Fe-Ni-OOH\u4e2dFe\/Ni-O\u7684\u952e\u957f\u4e0e\u5176\u5bf9\u5e94\u7684\u786b\u5316\u7269\u548c\u7852\u5316\u7269\u9884\u50ac\u5316\u5242\u4e2d\u7684Fe\/Ni-S, Fe\/Ni-Se\u7684\u952e\u957f\u5177\u6709\u660e\u663e\u7684\u5dee\u5f02\u3002<\/p>\n

\"\"<\/p>\n

Figure 2<\/strong>. k2-weighted Fourier transformed EXAFS at the Ni K<\/em>-edge of the D-Fe-Ni-OOH a), D(O)-Fe-Ni-OOH b), D(S)-Fe-Ni-OOH c) and D(Se)-Fe-Ni-OOH d) with EXAFS fitting. e) Wavelet transform for k2-weighted EXAFS signals at the Ni K<\/em>-edge of catalysts.<\/p>\n

\u5c0f\u6ce2\u53d8\u6362\u5206\u6790\u786e\u8ba4\u4e86\u50ac\u5316\u5242\u5728\u7ed3\u6784\u6f14\u53d8\u4e4b\u540e\u884d\u751f\u5f97\u5230\u7684\u7ed3\u6784\u4e3a\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u3002\u7814\u7a76\u56e2\u961f\u5bf9\u884d\u751f\u5f97\u5230\u7684\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u8fdb\u884cEXFAS\u62df\u5408\uff0c\u5f97\u51fa\u4e86\u8be6\u7ec6\u7684\u7ed3\u6784\u4fe1\u606f\u3002<\/p>\n

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Figure 3<\/strong>. Electrocatalytic performance. a) polarization curves of D-Fe-Ni-OOH, D(O)-Fe-Ni-OOH, D(S)-Fe-Ni-OOH and D(Se)-Fe-Ni-OOH in 1M KOH at a scanning rate of 5mV s-1<\/sup>. b) Comparison of the overpotential at a current density of 50 mA cm-2<\/sup> and the current density at an applied potential of 1.55 V vs. RHE for D-Fe-Ni-OOH, D(O)-Fe-Ni-OOH, D(S)-Fe-Ni-OOH and D(Se)-Fe-Ni-OOH. c) Tafel plots derived from the polarization curves in (a); d) EIS Nyquist plots. e) Comparison of the Debye-Waller factor (\u03c32<\/sup>) for catalysts extracted from EXAFS fitting results and the applied potential at a current density of 0.1 mA cm-2 ECSA.<\/p>\n

\u7535\u5316\u5b66\u6027\u80fd\u6d4b\u8bd5\u8868\u660e\uff0c\u76f8\u6bd4\u8f83\u4e8eD(O)-Fe-Ni-OOH\u548cD(S)-Fe-Ni-OOH\uff0cD(Se)-Fe-Ni-OOH\u5177\u6709\u66f4\u52a0\u51fa\u8272\u7684OER\u6d3b\u6027\u548c\u66f4\u5c0fTafel\u659c\u7387\uff0839.63 mv dec-1<\/sup>\uff09\u3002 \u5728\u7535\u6d41\u5bc6\u5ea6\u4e3a50 mA cm-2<\/sup>\u65f6\uff0c\u50ac\u5316\u5242\u5bf9\u6790\u6c27\u53cd\u5e94\u7684\u8fc7\u7535\u4f4d\u4e3a303 mV\u3002EXAFS\u5206\u6790\u8868\u660eD(Se)-Fe-Ni-OOH\u5177\u6709\u66f4\u9ad8\u7684\u7ed3\u6784\u65e0\u5e8f\u5ea6\uff08Fe-O path \u03c32<\/sup>=0.009 \u00c52<\/sup>; Ni-O path \u03c32<\/sup>=0.008 \u00c52<\/sup>\uff09\u3002<\/p>\n

\"\"<\/p>\n

Figure 4<\/strong>. a) Ni K<\/em>-edge XANES of D(S)-Ni-OOH and D(S)-Fe-Ni-OOH. b) k2-weighted Fourier transformed EXAFS at the Ni K<\/em>-edge of the D-Ni-OOH with EXAFS fitting. c) Debye-Waller factor (\u03c32<\/sup>) for D(S)-Fe-OOH, D(S)-Ni-OOH and D(S)-Fe-Ni-OOH extracted from EXAFS fitting results. d) PDF analysis for D-Fe-Ni-OOH and D(S)-Fe-Ni-OOH. Inset is a magnified view of the red box. e) HRTEM image of D(S)-Fe-Ni-OOH.<\/p>\n

\u4ee5\u786b\u5316\u7269\u4e3a\u4f8b\uff0c\u53cc\u91d1\u5c5eD(S)-Fe-Ni-OOH\u50ac\u5316\u5242\u4e0e\u5355\u91d1\u5c5eD(S)-Fe-OOH\u548cD(S)-Ni-OOH\u50ac\u5316\u5242\u7684XAFS\u5206\u6790\u8868\u660e\u53cc\u91d1\u5c5eD(S)-Fe-Ni-OOH\u50ac\u5316\u5242\u7684\u7ed3\u6784\u5177\u6709\u66f4\u9ad8\u7684\u65e0\u5e8f\u5ea6\u3002\u5bf9\u5206\u5e03\u51fd\u6570\u5206\u6790\u548c\u9ad8\u5206\u8fa8\u900f\u5c04\u7535\u955c\u663e\u793a\u4ece\u786b\u5316\u7269\u9884\u50ac\u5316\u5242\u884d\u751f\u51fa\u7684D(S)-Fe-Ni-OOH\u6bd4\u4ece\u76f4\u63a5\u5236\u5907\u5f97\u5230\u7684Fe-Ni-OOH\u884d\u751f\u51fa\u7684D-Fe-Ni-OOH\u50ac\u5316\u5242\u8868\u73b0\u51fa\u66f4\u9ad8\u7684\u7ed3\u6784\u65e0\u5e8f\u5ea6\u3002<\/p>\n

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Figure 5<\/strong>. In-situ XAFS characterizations. a) In situ XANES spectra recorded at the Ni K<\/em>-edge of Fe-Ni-S at different applied potentials from 1.23 to 2.03 V vs. RHE during the OER process. b) Oxidation state evolution of Ni species during the OER process. \u0394E denotes the K-edge position difference of samples in comparison with that of Ni foil. c) Wavelet transform of Ni K<\/em>-edge EXAFS spectra for Fe-Ni-S under various potentials during OER. d) Fourier transformed magnitudes of Ni K<\/em>-edge EXAFS spectra under various potentials during OER. e) k2-weighted Fourier transformed EXAFS at the Ni K<\/em>-edge of the Fe-Ni-S at 1.43 V vs. RHE with EXAFS fitting. f) The coordination number (CN) and bond length extracted from EXAFS fitting results. g) The Debye-Waller factor (\u03c32<\/sup>) for catalysts extracted from EXAFS fitting results.<\/p>\n

\u5229\u7528\u539f\u4f4dXAFS\u6280\u672f\u7814\u7a76\u4e86\u786b\u5316\u7269\u5728OER\u8fc7\u7a0b\u4e2d\u7684\u4ef7\u6001\u4ee5\u53ca\u7ed3\u6784\u65e0\u5e8f\u5ea6\u7684\u6f14\u53d8\u8fc7\u7a0b\u3002\u5728OER\u8fc7\u7a0b\u4e2d\uff0c\u50ac\u5316\u5242\u7684\u4ef7\u6001\u5728\u9010\u6e10\u589e\u9ad8\u5e76\u4e14\u50ac\u5316\u5242\u7531\u786b\u5316\u7269\u5411\uff08\u7f9f\u57fa\uff09\u6c22\u6c27\u5316\u7269\u8f6c\u53d8\u3002EXAFS\u62df\u5408\u7ed3\u679c\u8868\u660e\u5728\u7ed3\u6784\u6f14\u53d8\u7684\u8fc7\u7a0b\u4e2d\u5176\u65e0\u5e8f\u5ea6\uff08Debye-Waller factor\uff09\u9010\u6e10\u589e\u5927\u3002\u5c0f\u6ce2\u5206\u6790\u4e5f\u8bc1\u5b9e\u4e86\u4e0a\u8ff0\u7ed3\u6784\u6f14\u53d8\u7684\u8fc7\u7a0b\u3002<\/p>\n

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Figure 6<\/strong>. DFT calculations. a) TDOS of D-Fe-Ni-OOH, D(O)-Fe-Ni-OOH, D(S)-Fe-Ni-OOH and D(Se)-Fe-Ni-OOH. b) Free energy diagram for the OER over Ni sites for catalysts. c) Comparison of the theoretical calculated overpotentials and change in the octahedral distortion parameters of different DFT models. d) Linear scaling relationship for catalysts between the adsorption energy of OOH* versus the adsorption energy of OH* and between the adsorption energy of O* versus the adsorption energy of OH*. e) Calculated volcano plot of OER overpotential \u03b7 with \u0394GOH<\/sub> and \u0394GO<\/sub>-\u0394GOH<\/sub> as the descriptors.<\/p>\n

DFT\u8ba1\u7b97\u7ed3\u679c\u8868\u660e\u7ed3\u6784\u65e0\u5e8f\u548c\u5c40\u57df\u7ed3\u6784\u7578\u53d8\u80fd\u591f\u8c03\u63a7\u50ac\u5316\u5242\u7535\u5b50\u7ed3\u6784\u548c\u8c03\u63a7\u50ac\u5316\u5242\u7684\u53cd\u5e94\u70ed\u52a8\u529b\u5b66\uff0c\u589e\u5f3aOER\u6027\u80fd\u3002<\/p>\n

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

\u7efc\u4e0a\u6240\u8ff0\uff0c\u672c\u5de5\u4f5c\u9009\u53d6\u4e86\u8fc7\u6e21\u91d1\u5c5e\u6c27\u5316\u7269\uff0c\u786b\u5316\u7269\u548c\u7852\u5316\u7269\u7b49\u505a\u4e3a\u6a21\u578b\u9884\u50ac\u5316\u5242\uff0c\u7814\u7a76\u4e86\u5728OER\u8fc7\u7a0b\u4e2d\u5176\u7ed3\u6784\u65e0\u5e8f\u7684\u6f14\u53d8\u8fc7\u7a0b\u3002XAFS\u5206\u6790\u8868\u660e\u9884\u50ac\u5316\u5242\u4e0e\u539f\u4f4d\u884d\u751f\u50ac\u5316\u5242\u4e4b\u95f4\u7684\u952e\u957f\u5dee\u5f02\u4f1a\u4ea7\u751f\u66f4\u52a0\u65e0\u5e8f\u7684\u7ed3\u6784\uff0c\u663e\u793a\u51fa\u66f4\u5f3a\u7684\u6790\u6c27\u53cd\u5e94\u7535\u50ac\u5316\u6d3b\u6027\u3002\u672c\u5de5\u4f5c\u4ece\u7ed3\u6784\u65e0\u5e8f\u7684\u89d2\u5ea6\uff0c\u63ed\u793a\u6790\u6c27\u7535\u50ac\u5316\u7ed3\u6784\u6f14\u5316\u8fc7\u7a0b\u4e2d\u7ed3\u6784\u65e0\u5e8f\u4e0e\u6d3b\u6027\u7684\u76f8\u5173\u6027\uff0c\u6709\u671b\u4e3a\u76f8\u5173\u50ac\u5316\u5242\u7684\u5236\u5907\u4ee5\u53ca\u63ed\u793a\u5176\u7ed3\u6784-\u6027\u80fd\u5173\u7cfb\u63d0\u4f9b\u65b0\u7684\u601d\u8def\u3002<\/p>\n

\u539f\u6587\u8be6\u60c5<\/strong>\uff1aShouwei Zuo, Zhipeng Wu, Guikai Zhang, Cailing Chen, Yuanfu Ren, Lirong Zheng, Jing Zhang, Yu Han, Huabin Zhang. Correlating Structural Disorder in Metal (Oxy)hydroxides and Catalytic Activity in Electrocatalytic Oxygen Evolution. Angew. Chem. Int. Ed.2023, e202316762.<\/p>\n

https:\/\/doi.org\/10.1002\/anie.202316762<\/p>\n

\u672c\u6587\u7531Holmes\u4f9b\u7a3f<\/p>\n","protected":false},"excerpt":{"rendered":"

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