{"id":255849,"date":"2023-11-15T06:40:32","date_gmt":"2023-11-14T22:40:32","guid":{"rendered":"http:\/\/www.cailiaoniu.com\/?p=255849"},"modified":"2023-11-14T16:44:18","modified_gmt":"2023-11-14T08:44:18","slug":"kaust%e5%bc%a0%e5%8d%8e%e5%bd%ac%e8%af%be%e9%a2%98%e7%bb%84acs-nano-%e9%93%81%e5%8d%95%e5%8e%9f%e5%ad%90%e9%85%8d%e4%bd%8d%e7%bb%93%e6%9e%84%e7%9a%84%e7%94%b5%e5%ad%90%e6%89%b0%e5%8a%a8%e5%a2%9e","status":"publish","type":"post","link":"http:\/\/www.cailiaoniu.com\/?p=255849","title":{"rendered":"KAUST\u5f20\u534e\u5f6c\u8bfe\u9898\u7ec4ACS Nano: \u94c1\u5355\u539f\u5b50\u914d\u4f4d\u7ed3\u6784\u7684\u7535\u5b50\u6270\u52a8\u589e\u5f3a\u7535\u50ac\u5316\u56fa\u6c2e\u5408\u6210\u6c28"},"content":{"rendered":"

\u7b2c\u4e00\u4f5c\u8005\uff1a\u5e38\u5f6c\uff0c\u66f9\u81fb<\/p>\n

\u901a\u8baf\u4f5c\u8005\uff1a\u5f20\u534e\u5f6c\uff0cLuigi Cavallo<\/p>\n

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\u8bba\u6587DOI\uff1a10.1021\/acsnano.3c06212<\/p>\n

\"\"<\/p>\n

\u5168\u6587\u901f\u89c8<\/strong><\/p>\n

\u5728\u7535\u50ac\u5316\u56fa\u6c2e\u53cd\u5e94\u8fc7\u7a0b\u4e2d\uff0c\u5c40\u90e8\u7535\u5b50\u7ed3\u6784\u8c03\u8282\u5bf9\u4e8e\u63d0\u5347\u5355\u539f\u5b50\u7684\u50ac\u5316\u6548\u7387\u81f3\u5173\u91cd\u8981\u3002\u5bf9\u6b64\uff0c\u5f20\u534e\u5f6c\u6559\u6388\u548cLuigi Cavallo\u6559\u6388\u56e2\u961f\u901a\u8fc7\u8c03\u8282\u94c1\u6d3b\u6027\u4e2d\u5fc3\u7684\u81ea\u65cb\u6001\uff0c\u5b9e\u73b0\u4e86\u5bf9\u94c1\u5355\u539f\u5b50\u914d\u4f4d\u7ed3\u6784\u7684\u7535\u5b50\u6270\u52a8\u3002\u81ea\u65cb\u6781\u5316\u7684\u8dc3\u8fc1\u6709\u5229\u4e8e\u7535\u5b50\u7a7f\u900f\u6c2e\u7684\u53cd\u952e\u03c0\u8f68\u9053\uff0c\u6709\u6548\u6fc0\u6d3b\u6c2e\u5206\u5b50\uff0c\u4ece\u800c\u5b9e\u73b0\u4e86115 \u03bcg h-1<\/sup>\u00a0mg-1<\/sup>cat<\/sub>\u7684\u6c28\u4ea7\u7387\u3002\u539f\u4f4d\u5149\u8c31\u7814\u7a76\u548c\u7406\u8bba\u8ba1\u7b97\u8868\u660e\uff0c\u787c\u914d\u4f4d\u7684\u5f15\u5165\u53ef\u4ee5\u8c03\u8282Nx<\/sub>Hy<\/sub>\u4e2d\u95f4\u4f53\u5728Fe\u4e2d\u5fc3\u7684\u5438\u9644\u80fd\u3002FeN2<\/sub>B2<\/sub>\u4f4d\u70b9\u6709\u5229\u4e8eNNH*\u4e2d\u95f4\u4ea7\u7269\u7684\u5f62\u6210\uff0c\u964d\u4f4e\u4e86\u901f\u7387\u51b3\u5b9a\u6b65\u9aa4\u7684\u80fd\u91cf\u52bf\u5792\uff0c\u56e0\u6b64\u5177\u6709\u4f18\u5f02\u7684\u56fa\u6c2e\u6027\u80fd\u3002<\/p>\n

\u672c\u6587\u4eae\u70b9<\/strong><\/p>\n

1.\u672c\u5de5\u4f5c\u901a\u8fc7\u5f15\u5165Lewis\u9178\u787c\u914d\u4f4d\u4f4d\u70b9\uff08FeN2<\/sub>B2<\/sub>\uff09\u5b9e\u73b0Fe\u5355\u539f\u5b50\u4f4d\u70b9\u7b2c\u4e00\u914d\u4f4d\u5c42\u7684\u7535\u5b50\u6270\u52a8\u3002<\/p>\n

2.d<\/i><\/em>\u8f68\u9053\u7ed3\u6784\u8c03\u63a7\u4fc3\u8fdb\u4e86\u6c2e\u5438\u9644\uff0c\u540c\u65f6\u52a0\u901f\u4e86Nx<\/sub>Hy<\/sub>\u4e2d\u95f4\u4f53\uff08*N2<\/sub>\u2192 *NNH\uff09\u7684\u8868\u9762\u53cd\u5e94\u52a8\u529b\u5b66\u3002<\/p>\n

3.\u5177\u6709\u4f18\u5316\u81ea\u65cb\u6784\u578b\u548c\u7535\u5b50\u79bb\u57df\u7684\u94c1\u6d3b\u6027\u4f4d\u70b9\u83b7\u5f97\u4e86\u8f83\u597d\u7684\u56fa\u6c2e\u6027\u80fd\u3002<\/p>\n

\u56fe\u6587\u89e3\u6790<\/strong><\/p>\n

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Figure 1.<\/b><\/strong>\u00a0Theoretical studies of electronic perturbation. (a) Scheme of the electronic perturbation of isolated Fe coordination sphere for nitrogen fixation. (b) The structure and charge density differences of FeN4<\/sub>-C structures and (c) FeN2<\/sub>B2<\/sub>-C structure. (d) The structure and HOMO\/LUMO charge density distributions of FeN4<\/sub>-C with adsorbed nitrogen and (e)FeN2<\/sub>B2<\/sub>-C structures with adsorbed nitrogen. (f) Calculated free energy diagram of the nitrogen reduction reaction mechanism on FeN4<\/sub>-C and (g) FeN2<\/sub>B2<\/sub>-C.<\/p>\n

\u672c\u5de5\u4f5c\u9996\u5148\u4ee5FeN4<\/sub>-C\u4f53\u7cfb\u4e3a\u7ed3\u6784\u8c03\u63a7\u6a21\u677f\uff0c\u901a\u8fc7\u52a0\u5165\u989d\u5916\u7684\u787c\u539f\u5b50\u6765\u53d6\u4ee3\u4e0e\u94c1\u914d\u4f4d\u7684N\u539f\u5b50\uff0c\u4f7f\u5f97\u4e2d\u5fc3\u94c1\u539f\u5b50\u4e0e\u90bb\u8fd1\u914d\u4f4d\u539f\u5b50\u4e4b\u95f4\u5b58\u5728\u66f4\u5f3a\u7684\u7535\u5b50\u8026\u5408\u3002\u5409\u5e03\u65af\u81ea\u7531\u80fd\u5206\u6790\u6a21\u62dfFeN4<\/sub>-C\u548cFeN2<\/sub>B2<\/sub>-C\u5bf9N2\u7684\u5438\u9644\u548c\u6d3b\u5316\u884c\u4e3a\u3002\u5f15\u5165\u7684Lewis\u9178\u787c\u914d\u4f4d\u4f18\u5316\u4e86N2<\/sub>-Fe-B2<\/sub>\u4f4d\u70b9\u7684\u7535\u5b50\u7ed3\u6784\uff0c\u6c22\u5316\u80fd\u5792\u660e\u663e\u964d\u4f4e\uff0c\u66f4\u6709\u5229\u4e8e\u6c2e\u4e2d\u95f4\u4f53\u7684\u6355\u83b7\u3002<\/p>\n

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Figure 2.<\/b><\/strong>\u00a0Physicochemical properties of FeN2<\/sub>B2<\/sub>-C.\u00a0(a) SEM image, (b) TEM image, (c) room-temperature 57<\/sup>Fe M\u00f6ssbauer spectrum, (d) high-resolution AC-HAADF-STEM image, (e) pseudocolor surface plot of the selected area, (f) EELS spectra and (g) EDX mapping images of FeN2<\/sub>B2<\/sub>-C. The scale bar of Figure 2g is 50 nm.<\/p>\n

\u901a\u8fc7\u6c34\u51dd\u80f6\u7145\u70e7\u65b9\u6cd5\u5408\u6210\u4e86\u5177\u6709\u4e0d\u540c\u914d\u4f4d\u4f4d\u70b9\u7684\u94c1\u5355\u539f\u5b50\u50ac\u5316\u5242\u3002\u7403\u5dee\u7535\u955c\u53ca\u7a46\u65af\u5821\u5c14\u8c31\u8bc1\u5b9e\u4e86\u94c1\u5355\u539f\u5b50\u7684\u6210\u529f\u5236\u5907\u3002EELS\u8c31\u56fe\u660e\u663e\u663e\u793a\u51fa\u6e05\u6670\u7684B\u3001C\u3001N\u548cFe\u4fe1\u53f7\u3002EDX mapping\u8bc1\u5b9eFe\u5143\u7d20\u7684\u5b58\u5728\u53ca\u5176\u5728\u50ac\u5316\u5242\u8868\u9762\u7684\u5747\u5300\u5206\u5e03\u3002<\/p>\n

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Figure 3.<\/b><\/strong>\u00a0Chemical structures of FeN2<\/sub>B2<\/sub>-C. (a) High-resolution XPS spectra of B1s, (b) N1s and (c) Fe 2p. (d) Fe K-edge XANES spectra. (e) k2<\/sup>-weighted FT-EXAFS curves at the Fe K-edge. (f) WT contour plots of the EXAFS signal for FeN2<\/sub>B2<\/sub>-C, FeN4<\/sub>-C, Fe2<\/sub>O3,<\/sub>\u00a0and Fe foil reference samples, respectively. (g) FT-EXAFS fitting curves in R space\u00a0of FeN2<\/sub>B2<\/sub>-C. (h) The Fe K-edge XANES experimental spectrum of FeN2<\/sub>B2<\/sub>-C and the corresponding theoretical spectrum calculated with the depicted structure.<\/p>\n

\u540c\u6b65\u8f90\u5c04\u6280\u672f\u8fdb\u4e00\u6b65\u8868\u5f81\u4e86\u94c1\u5355\u539f\u5b50\u7684\u5177\u4f53\u914d\u4f4d\u7ed3\u6784\u3002\u94c1\u7269\u79cd\u5728\u78b3\u8868\u9762\u662f\u4ee5\u5355\u5206\u6563\u5f62\u5f0f\u5b58\u5728\u7684\u3002\u5bf9\u6bd4\u53c2\u7167\u6837\u54c1\uff0cFeN2<\/sub>B2<\/sub>-C\u5728\u7b2c\u4e00\u58f3\u5c42\u6709\u660e\u663e\u7684Fe-N\u548cFe-B\u952e\u5cf0\u3002\u7ed3\u5408\u5b9e\u9a8c\u8c31\u56fe\u548c\u7406\u8bba\u6a21\u62df\u8c31\u56fe\uff0c\u53ef\u4ee5\u786e\u5b9aFeN2<\/sub>B2<\/sub>-C\u4e2d\u7684\u94c1\u539f\u5b50\u4e3b\u8981\u5f62\u6210\u5177\u6709\u72ec\u7279\u7684N2-<\/sub>Fe-B2<\/sub>\u914d\u4f4d\u6784\u578b\u7684\u914d\u4f4d\u952e\u3002<\/p>\n

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Figure 4.<\/b><\/strong>\u00a0Electrochemical performance of FeN2<\/sub>B2<\/sub>-C.\u00a0(a) Magnetic susceptibility of FeN2<\/sub>B2<\/sub>-C.\u00a0(b)\u00a0N2<\/sub>-TPD patterns of FeN2<\/sub>B2<\/sub>-C, FeN4<\/sub>-C, and Fe-C, respectively.\u00a0(c) Linear sweep voltammetry curves in N2<\/sub>\u00a0and Ar-saturated neutral solutions. (d) Ammonia yield rate and Faradaic efficiency at the corresponding potentials. (e) Electrochemical nitrogen fixation performance at -0.2 V vs. RHE, (f) Bode phase plots\u00a0of the in-situ<\/i><\/em>\u00a0EIS, (g) H2<\/sub>\u00a0yields, and (h) H2<\/sub>\u00a0selectivity of FeN2<\/sub>B2<\/sub>-C, FeN4<\/sub>-C, and Fe-C, respectively. (i) The comparison of the electrochemical nitrogen fixation performance of FeN2<\/sub>B2<\/sub>-C and reported representative work.<\/p>\n

\u7ed3\u5408\u78c1\u5316\u7387\u5206\u6790\u548c\u5316\u5b66\u6d17\u8131\u9644\u6d4b\u8bd5\u8bc1\u660e\uff0c\u81ea\u65cb\u6001\u8c03\u6574\u540e\u7684\u94c1\u5355\u539f\u5b50\u6750\u6599\u8868\u73b0\u51fa\u4e86\u8f83\u5f3a\u7684\u6c2e\u5438\u9644\u80fd\u529b\u3002\u968f\u540e\u7684\u50ac\u5316\u6027\u80fd\u6d4b\u8bd5\u8868\u660e\uff0cFeN2<\/sub>B2<\/sub>-C\u5177\u6709\u4f18\u4e8eFeN4<\/sub>C\u7684\u7535\u50ac\u5316\u6c2e\u8fd8\u539f\u5408\u6210\u6c28\u6d3b\u6027\uff0c\u5b9e\u73b0\u4e86115 \u03bcg h-1<\/sup>\u00a0mg-1<\/sup>cat<\/sub>\u7684\u6c28\u4ea7\u7387\u548c24.8 %\u7684\u6cd5\u62c9\u7b2c\u6548\u7387\u3002\u539f\u4f4d\u7535\u5316\u5b66\u963b\u6297\u8c31\u7684\u4f4e\u9891\u533a(10-1<\/sup>~101<\/sup>\u00a0Hz)\u5bf9\u5e94\u4e8e\u975e\u5747\u5300\u7535\u8377\u5206\u5e03\uff0c\u8868\u660e\u7535\u6781\u754c\u9762\u4e0a\u5b58\u5728\u53cd\u5e94\u4e2d\u95f4\u4f53\u3002\u5f15\u5165Lewis\u9178\u787c\u914d\u4f4d\u540e\uff0cFeN2<\/sub>B2<\/sub>-C\u5728\u4f4e\u9891\u533a\u76f8\u503c\u964d\u4f4e\uff0c\u8fdb\u4e00\u6b65\u8868\u73b0\u51fa\u589e\u5f3a\u7684\u6c2e\u8fd8\u539f\u6027\u80fd\u3002<\/p>\n

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Figure 5.<\/b><\/strong>\u00a0The confirmation and mechanism exploration of nitrogen fixation on FeN2<\/sub>B2<\/sub>-C.<\/i><\/em>\u00a0(a) 1<\/sup>H NMR spectra of both 14<\/sup>NH4<\/sub>+<\/sup>\u00a0and 15<\/sup>NH4<\/sub>+<\/sup>\u00a0obtained from the nitrogen reduction on FeN2<\/sub>B2<\/sub>-C using 14<\/sup>N2<\/sub>\u00a0or 15<\/sup>N2<\/sub>\u00a0as the nitrogen source, respectively.\u00a0(b) 1<\/sup>H NMR spectra of the electrolyte with different electrolysis times under a 15<\/sup>N2<\/sub>\u00a0atmosphere with maleic acid as internal standard.\u00a0(c) Calculated ammonia yield using colorimetric, NMR quantifications, and ion chromatography methods. The error bars correspond to the standard deviations (n\u2009=\u20093) of measurements taken under the same conditions. (d) in situ<\/i><\/em>\u00a0Raman spectra and (e) in situ<\/i><\/em>\u00a0FTIR spectra of FeN2<\/sub>B2<\/sub>-C collected with different electrolysis times under an N2<\/sub>\u00a0atmosphere. (f) The FTIR spectrum of FeN2<\/sub>B2<\/sub>-C after 2 hours\u2019 reaction.<\/p>\n

\u901a\u8fc7\u5305\u542b\u540c\u4f4d\u7d20\u6d4b\u8bd5\u5728\u5185\u7684\u4e0d\u540c\u68c0\u6d4b\u65b9\u6cd5\u5b9a\u91cf\u4e86FeN2<\/sub>B2<\/sub>-C\u7684\u7535\u5316\u5b66\u5408\u6210\u6c28\u4ea7\u7269\u3002\u5f15\u5165\u539f\u4f4d\u62c9\u66fc\u53ca\u539f\u4f4d\u7ea2\u5916\u5149\u8c31\u6cd5\u6765\u68c0\u6d4b\u7535\u5316\u5b66\u56fa\u6c2e\u8fc7\u7a0b\u4e2d\u7684\u53cd\u5e94\u4ea7\u7269\u53ca\u53cd\u5e94\u4e2d\u95f4\u4f53\u3002\u5728FeN2<\/sub>B2<\/sub>-C\u9634\u6781\u8868\u9762\uff0cNH3<\/sub>\u53ca*N2<\/sub>Hy<\/sub>\u4e2d\u95f4\u4f53\u7684\u51fa\u73b0\u4e3a\u6c2e\u8fd8\u539f\u7684\u53d1\u751f\u63d0\u4f9b\u4e86\u5206\u5b50\u6c34\u5e73\u7684\u8bc1\u636e\u3002<\/p>\n

\u603b\u7ed3\u4e0e\u5c55\u671b<\/strong><\/p>\n

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\u901a\u8baf\u4f5c\u8005\u7b80\u4ecb<\/strong><\/p>\n

\u5f20\u534e\u5f6c<\/b><\/strong>\u6559\u6388\uff1a2020\u5e7412\u6708\u52a0\u5165\u963f\u535c\u675c\u62c9\u56fd\u738b\u79d1\u6280\u5927\u5b66\uff08KAUST\uff09, \u5316\u5b66\u79d1\u5b66\u7cfb\uff0c\u62c5\u4efb\u72ec\u7acbPI, \u535a\u58eb\u751f\u5bfc\u5e08\u3002\u5f20\u534e\u5f6c\u535a\u58eb\u4e8e2013\u5e74\u4e8e\u4e2d\u56fd\u79d1\u5b66\u9662\u83b7\u5f97\u535a\u58eb\u5b66\u4f4d\uff0c\u540c\u5e74\u4e8e\u4e2d\u56fd\u79d1\u5b66\u9662\u62c5\u4efb\u52a9\u7406\u7814\u7a76\u5458\u30022014\u5e74\u81f32017\u5e74\u4e8e\u65e5\u672c\u56fd\u7acb\u7269\u8d28\u7814\u7a76\u6240\u8fdb\u884c\u535a\u58eb\u540e\u7814\u7a76\u3002\u5e76\u4e8e2017\u5e743\u6708\u4efd\u52a0\u5165\u65b0\u52a0\u5761\u5357\u6d0b\u7406\u5de5\u5927\u5b66(Research fellow)\u3002\u957f\u671f\u81f4\u529b\u4e8e\u6784\u7b51\u5355\u539f\u5b50\u50ac\u5316\u5242\u5728\u80fd\u6e90\u8f6c\u5316\u4e0e\u73af\u5883\u4f18\u5316\u9886\u57df\u7684\u5e94\u7528\u3002\u76ee\u524d\u5df2\u53d1\u8868\u8bba\u6587\/\u4e13\u8457\u7ae0\u8282130\u4f59\u7bc7\uff0c\u6587\u7ae0\u5f15\u7528\u6b21\u657014000\u4f59\u6b21\uff0cH\u56e0\u5b5060\uff0c\u4e3a2020\u5e74\u81f32023\u5e74\u79d1\u777f\u552f\u5b89\u5168\u7403\u9ad8\u88ab\u5f15\u5b66\u8005\u3002\u5176\u4e2d\u591a\u7bc7\u6587\u7ae0\u4ee5\u7b2c\u4e00\/\u901a\u8baf\u4f5c\u8005\u53d1\u8868\u5728Sci. Adv., Joule, Adv. Mater., Energy Environ. Sci., Angew. Chem. Int. Ed., J. Am. Chem. Soc., Adv. Energy Mater., Adv. Funct. Mater., ACS Nano, Nano Energy\u7b49\u56fd\u9645\u8457\u540d\u671f\u520a\u3002<\/p>\n

\u7b2c\u4e00\u4f5c\u8005\u7b80\u4ecb<\/strong><\/p>\n

\u5e38\u5f6c<\/b><\/strong>\u535a\u58eb\uff1a2020\u5e74\u4e8e\u5c71\u4e1c\u5927\u5b66\u83b7\u5f97\u535a\u58eb\u5b66\u4f4d\u30022020~2022\u5e74\uff0c\u6d4e\u5357\u5927\u5b66\/\u52a0\u62ff\u5927\u56fd\u7acb\u79d1\u5b66\u9662\u535a\u58eb\u540e\uff08\u5408\u4f5c\u5bfc\u5e08\uff1a\u5468\u4f1f\u5bb6\u6559\u6388\u3001\u5b59\u4e66\u4f1a\u9662\u58eb\uff09\u30022022\u5e74\u81f3\u4eca\uff0c\u963f\u535c\u675c\u62c9\u56fd\u738b\u79d1\u6280\u5927\u5b66\u535a\u58eb\u540e\uff08\u5408\u4f5c\u5bfc\u5e08\uff1a\u5f20\u534e\u5f6c\u6559\u6388\uff09\u3002\u4e3b\u8981\u4ece\u4e8b\u7535\u50ac\u5316\u78b3\u3001\u6c2e\u5faa\u73af\u53cd\u5e94\u673a\u7406\u7814\u7a76\uff0c\u4ee5\u7b2c\u4e00\u6216\u901a\u8baf\u4f5c\u8005\u5728Energy Environ. Sci., ACS Energy Lett., ACS Nano, Chem, Nano Energy, Appl. Catal. B-Environ.\u7b49\u671f\u520a\u53d1\u8868SCI\u6536\u5f55\u8bba\u658718\u7bc7\uff0cH\u56e0\u5b5021\u3002<\/p>\n

\u8bfe\u9898\u7ec4\u4ecb\u7ecd<\/strong><\/p>\n

https:\/\/acse.kaust.edu.sa\/<\/b><\/strong><\/p>\n

Advanced Catalysis of Sustainable Energy (ACSE), headed by Huabin Zhang (Assistant Professor of Chemistry) in the KAUST Catalysis Center.<\/p>\n

Lab of ACSE focuses on the development of single-atom catalysts with the particular configuration for sustainable energy conversion, including photocatalysis, electrocatalysis, and thermal catalysis. Our research also extends to the operando investigation for monitoring the structural evolution of the reactive centers, as well as the mutual interaction between the reactive center and reactant in the catalytic process.<\/p>\n","protected":false},"excerpt":{"rendered":"

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