{"id":221308,"date":"2021-05-01T06:03:24","date_gmt":"2021-04-30T22:03:24","guid":{"rendered":"\/\/m.iemloyee.com\/?p=221308"},"modified":"2021-04-30T21:03:42","modified_gmt":"2021-04-30T13:03:42","slug":"%e9%99%95%e8%a5%bf%e5%b8%88%e5%a4%a7%e5%88%98%e5%bf%a0%e6%96%87%e5%8e%a6%e5%a4%a7%e7%8e%8b%e9%87%8e%e8%a5%bf%e5%ae%89%e4%ba%a4%e5%a4%a7%e5%b8%b8%e6%98%a5%e7%84%b6%e5%9b%a2%e9%98%9fnat-commun","status":"publish","type":"post","link":"\/\/m.iemloyee.com\/?p=221308","title":{"rendered":"\u9655\u897f\u5e08\u5927\u5218\u5fe0\u6587&\u53a6\u5927\u738b\u91ce&\u897f\u5b89\u4ea4\u5927\u5e38\u6625\u7136\u56e2\u961fNat. Commun.\uff1a\u6c2e\u5316\u9553\u50ac\u5316CO2\u76f4\u63a5\u52a0\u6c22\u5408\u6210\u4e8c\u7532\u919a"},"content":{"rendered":"

\u3010\u5f15\u8a00\u3011<\/strong><\/p>\n

\u73b0\u4ee3\u793e\u4f1a\u56e0\u4f7f\u7528\u5316\u77f3\u71c3\u6599\u6392\u653e\u4e86\u5927\u91cf\u7684CO2<\/sub>\uff0c\u7531\u4e8e\u5176\u6e29\u5ba4\u6548\u5e94\uff0c\u5f15\u53d1\u4e86\u4e0d\u5229\u7684\u6c14\u5019\u53d8\u5316\u3002\u901a\u8fc7\u98ce\u80fd\u6216\u592a\u9633\u80fd\u7b49\u53ef\u518d\u751f\u80fd\u6e90\u63d0\u4f9b\u53ef\u6301\u7eed\u7684H2<\/sub>\u5c06CO2<\/sub>\u52a0\u6c22\u4e3a\u78b3\u6c22\u5316\u5408\u7269\uff08HCs\uff0c\u5982CH4<\/sub>\u3001C2<\/sub>-C4<\/sub>\u70ef\u70c3\u548c\u6c7d\u6cb9\uff09\u548c\u542b\u6c27\u5316\u5408\u7269\uff08\u7532\u9187\u3001\u4e59\u9187\u3001\u4e59\u9178\u3001\u4e8c\u7532\u919a\uff08DME\uff09\u7b49\uff09\uff0c\u8fd9\u53ef\u4ee5\u5b9e\u73b0\u53ef\u6301\u7eed\u5730\u5c06\u53ef\u518d\u751f\u8d44\u6e90\u8f6c\u6362\u6210\u5316\u5b66\u54c1\u548c\u71c3\u6599\u3002\u56e0\u6b64\uff0c\u8fd1\u5e74\u6765\u5c06CO2<\/sub>\u52a0\u6c22\u4e3aCO\u3001HCs\u548c\u542b\u6c27\u5316\u5408\u7269\u65b9\u9762\u53d6\u5f97\u4e86\u91cd\u5927\u8fdb\u5c55\u3002\u5728\u8fd9\u4e9b\u4ea7\u54c1\u4e2d\uff0cDME\u662f\u4e00\u79cd\u65e0\u6bd2\u3001\u65e0\u81f4\u764c\u3001\u65e0\u8150\u8680\u6027\u7684\u91cd\u8981\u5de5\u4e1a\u5316\u5b66\u54c1\uff0c\u7528\u4e8e\u5316\u5986\u54c1\u7684\u4fc3\u8fdb\u5242\uff0c\u662f\u4e00\u79cd\u6781\u6709\u524d\u9014\u7684\u8d85\u6e05\u6d01\u71c3\u6599\uff0c\u53ef\u66ff\u4ee3\u6db2\u5316\u77f3\u6cb9\u6c14\u548c\u67f4\u6cb9\u3002\u66f4\u91cd\u8981\u7684\u662f\uff0c\u4eceCO2<\/sub>\u52a0\u6c22\u5408\u6210DME\u663e\u793a\u51fa\u6700\u9ad8\u7684\u6548\u7387\uff0c\u5373\u5728DME\u7684\u5408\u6210\u8fc7\u7a0b\u4e2d\uff0c97%\u7684\u80fd\u91cf\u88ab\u50a8\u5b58\u5728DME\u4e2d\uff0c\u8fd9\u6bd4\u50a8\u5b58\u5728\u78b3\u6c22\u5316\u5408\u7269\u6216\u9ad8\u7ea7\u9187\u4e2d\u7684\u80fd\u91cf\u8981\u9ad8\u3002\u901a\u5e38\u60c5\u51b5\u4e0b\uff0c\u91d1\u5c5e\/\u56fa\u4f53\u9178\u6742\u5316\u50ac\u5316\u5242\u901a\u8fc7\u4e00\u6b65\u8026\u5408\u8fc7\u7a0b\u5c06CO2<\/sub>\u52a0\u6c22\u4e3aDME\u3002\u5728\u8fd9\u79cd\u60c5\u51b5\u4e0b\uff0c\u91d1\u5c5e\u57fa\u50ac\u5316\u5242\uff0c\u5982Cu\/ZnO\/Al2<\/sub>O3<\/sub>\u50ac\u5316CO2<\/sub>\u52a0\u6c22\u4e3a\u7532\u9187\uff0c\u800c\u9178\u4f4d\u70b9\uff08\u5982HZSM-5\uff09\u4f7f\u4e2d\u95f4\u7532\u9187\u8131\u6c34\u5f62\u6210DME\u3002\u6c2e\u5316\u9553\uff08GaN\uff09\u4f5c\u4e3aIII\u65cf\u6c2e\u5316\u7269\u7684\u91cd\u8981\u6210\u5458\uff0c\u662f\u4e00\u79cd\u70ed\u529b\u5b66\u7a33\u5b9a\u7684\u7ea4\u950c\u77ff\u7ed3\u6784\u7684\u5bbd\u7981\u5e26\u534a\u5bfc\u4f53\uff0c\u5176\u57fa\u672c\u5e26\u9699\u80fd\u91cf\u4e3a3.4 eV\uff0c\u7531\u4e8e\u5176\u72ec\u7279\u7684\u7535\u5b50\u548c\u5149\u5b66\u7279\u6027\uff0c\u88ab\u4f5c\u4e3a\u4e00\u79cd\u9769\u547d\u6027\u7684\u6750\u6599\u8fdb\u884c\u5b9a\u91cf\u7814\u7a76\u3002\u5728\u50ac\u5316\u5e94\u7528\u65b9\u9762\u7531\u4e8eGaN\u5177\u6709\u8f83\u9ad8\u7684\u5316\u5b66\u548c\u70ed\u7a33\u5b9a\u6027\uff0c\u5b83\u4f5c\u4e3a\u4e00\u79cd\u5149\u50ac\u5316\u5242\u88ab\u8d8a\u6765\u8d8a\u591a\u5730\u7814\u7a76\u3002\u8fd1\u5e74\u6765\uff0c\u4eba\u4eec\u53d1\u73b0GaN\u5728\u7532\u70f7\u7b49\u8f7b\u8d28\u70f7\u70c3\u7684\u975e\u6c27\u5316\u82b3\u6784\u5316\u53cd\u5e94\u4e2d\u5177\u6709\u6d3b\u6027\u548c\u9009\u62e9\u6027\uff0c\u8fd9\u8868\u660e\u5176\u5bf9C-H\u952e\u7684\u6d3b\u5316\u5177\u6709\u50ac\u5316\u80fd\u529b\u3002\u6b64\u5916\uff0c\u6839\u636e\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\uff08DFT\uff09\u8ba1\u7b97\uff0cGaN\u5177\u6709\u9178\u6027\u8d28\u3002\u56e0\u6b64\uff0c\u8003\u8651\u5230\u8fd9\u4e9b\u6027\u8d28\u4ee5\u53ca\u5bf9CO2<\/sub>\u8f6c\u5316\u4e3aDME\u7684\u673a\u7406\u7684\u7406\u89e3\uff0cGaN\u6709\u671b\u6210\u4e3aCO2<\/sub>\u76f4\u63a5\u52a0\u6c22\u4e3aDME\u7684\u4e0d\u540c\u7c7b\u578b\u50ac\u5316\u5242\u3002<\/p>\n

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

\u8fd1\u65e5\uff0c\u5728\u9655\u897f\u5e08\u8303\u5927\u5b66\u5218\u5fe0\u6587<\/b><\/strong>\u6559\u6388\u3001\u53a6\u95e8\u5927\u5b66\u738b\u91ce\u6559\u6388<\/b><\/strong>\u548c\u897f\u5b89\u4ea4\u901a\u5927\u5b66\u5e38\u6625\u7136\u6559\u6388<\/b><\/strong>\u56e2\u961f\u7b49\u4eba\u5e26\u9886\u4e0b\uff0c\u62a5\u9053\u4e86\u6c2e\u5316\u9553\uff08GaN\uff09\u50ac\u5316CO2<\/sub>\u76f4\u63a5\u52a0\u6c22\u4e3a\u4e8c\u7532\u919a\uff08DME\uff09\uff0c\u5176\u975eCO\u9009\u62e9\u6027\u7ea6\u4e3a80%\u3002\u5c3d\u7ba1\u4ea7\u54c1\u7684\u5206\u5e03\u975e\u5e38\u76f8\u4f3c\uff0c\u4f46GaN\u5bf9CO2<\/sub>\u52a0\u6c22\u7684\u6d3b\u6027\u6bd4\u5bf9CO\u52a0\u6c22\u7684\u6d3b\u6027\u9ad8\u5f97\u591a\u3002\u7a33\u6001\u548c\u77ac\u6001\u5b9e\u9a8c\u7ed3\u679c\u3001\u5149\u8c31\u7814\u7a76\u548c\u5bc6\u5ea6\u6cdb\u51fd\u7406\u8bba\u8ba1\u7b97\u4e25\u683c\u5730\u63ed\u793a\u4e86DME\u662f\u901a\u8fc7\u7532\u57fa\u548c\u7532\u9178\u76d0\u7684\u4e2d\u95f4\u4f53\u4ea7\u751f\u7684\uff0c\u5b83\u4eec\u5728GaN\u7684\u4e0d\u540c\u6676\u9762\u4e0a\u4ee5\u76f8\u4f3c\u7684\u6d3b\u5316\u80fd\u5f62\u6210\u3002\u8fd9\u4e0e\u4f20\u7edf\u7684\u901a\u8fc7\u7532\u9187\u4e2d\u95f4\u4f53\u5728\u6742\u5316\u50ac\u5316\u5242\u4e0a\u5408\u6210DME\u7684\u65b9\u6cd5\u6709\u672c\u8d28\u533a\u522b\u3002\u672c\u5de5\u4f5c\u63d0\u4f9b\u4e86\u4e00\u79cd\u4e0d\u540c\u7684\u50ac\u5316\u5242\uff0c\u80fd\u591f\u5c06CO2<\/sub>\u76f4\u63a5\u52a0\u6c22\u4e3aDME\uff0c\u4ece\u800c\u4e30\u5bcc\u4e86CO2<\/sub>\u8f6c\u5316\u7684\u5316\u5b66\u8fc7\u7a0b\u3002\u8be5\u6210\u679c\u4ee5\u9898\u4e3a\u201cGallium nitride catalyzed the direct hydrogenation of carbon dioxide to dimethyl ether as primary product\u201d<\/b><\/strong>\u53d1\u8868\u5728\u4e86Nat. Commun.<\/b><\/strong>\u4e0a\u3002<\/p>\n

\u3010\u56fe\u6587\u5bfc\u8bfb\u3011<\/strong><\/p>\n

\u56fe<\/strong>1 \u5546\u7528GaN\u5728\u4e0d\u540c\u6e29\u5ea6\u4e0b\u5bf9CO<\/strong>2<\/sub><\/strong>\u6c22\u5316\u7684\u50ac\u5316\u6027\u80fd<\/strong>\"\"<\/p>\n

a\uff09DME\uff08STYDME\uff09\u7684CO2<\/sub>\u8f6c\u5316\u7387\u3001\u4e0d\u540c\u4ea7\u7269\u7684\u9009\u62e9\u6027\u548c\u65f6\u7a7a\u4ea7\u7387\u3002<\/p>\n

b\uff09\u78b3\u6c22\u5316\u5408\u7269\uff08HCs\uff09\u548c\u542b\u6c27\u5316\u5408\u7269\u5206\u5e03\u7684\u65e0CO\u5206\u5e03\u3002\u53cd\u5e94\u6761\u4ef6\uff1aP\uff1d2.0 MPa\uff0cH2<\/sub>\/CO2<\/sub>=3\uff0c\u6c14\u65f6\u7a7a\u901f\uff1d3000 mL g-1<\/sup>\u00a0h-1<\/sup>\uff0c\u53cd\u5e94\u65f6\u95f4=40 h\u3002\u76f8\u5bf9\u504f\u5dee\u7684\u8bef\u5dee\u68d2\u57285\uff05\u4ee5\u5185\u3002<\/p>\n

\u56fe<\/strong>2 GaN-26.6\u50ac\u5316\u5242\u7684\u7ed3\u6784\u8868\u5f81<\/strong>\"\"<\/p>\n

a\uff09X\u5c04\u7ebf\u884d\u5c04\u56fe\u3002<\/p>\n

b\uff09\u900f\u5c04\u7535\u955c\u56fe\u50cf\u3002<\/p>\n

c\uff09\u9009\u5b9a\u533a\u57df\u7684\u7535\u5b50\u884d\u5c04\u56fe\u3002<\/p>\n

\u56fe<\/strong>3 GaN\u6676\u4f53\u6027\u8d28\u5bf9\u50ac\u5316\u6027\u80fd\u7684\u5f71\u54cd<\/strong>\"\"<\/p>\n

a\uff09\u5c3a\u5bf8\u6548\u5e94\u5bf9\u4e0d\u540c\u4ea7\u7269CO2<\/sub>\u8f6c\u5316\u7387\u3001\u9009\u62e9\u6027(Sele.)\u548c\u4e8c\u7532\u919a(STYDME)\u7a7a\u65f6\u4ea7\u7387\u7684\u5f71\u54cd\u3002<\/p>\n

b\uff09\u7528\u4e8eCO2<\/sub>\u52a0\u6c22\u7684\u78b3\u6c22\u5316\u5408\u7269\uff08HCs\uff09\u548c\u542b\u6c27\u5316\u5408\u7269\u7684\u65e0CO\u5206\u5e03\u3002\u00a0<\/p>\n

c\u2013h\uff09\u5e26\u6709STYDME\u7684\uff08001\uff09\u3001\uff08110\uff09\u548c\uff08100\uff09\u5e73\u9762\u7684\u8d28\u6784\u7cfb\u6570\uff08TC\uff09\u4e0eCO\u7684\u65f6\u7a7a\u4ea7\u7387\uff08STYCO\uff09\u4e4b\u95f4\u7684\u76f8\u5173\u6027\u3002\u53cd\u5e94\u6761\u4ef6\uff1aP = 2.0 MPa, T = 360\u00b0C, H2<\/sub>\/CO2<\/sub>\u00a0= 2\u62163\uff0c\u6c14\u4f53\u6bcf\u5c0f\u65f6\u7a7a\u901f= 3000ml g\u22121<\/sup>\u00a0h\u22121<\/sup>\uff0c\u6d41\u4e0a\u65f6\u95f4= 40h\u3002\u76f8\u5bf9\u504f\u5dee\u7684\u8bef\u5dee\u68d2\u57285%\u4ee5\u5185\u3002<\/p>\n

\u56fe<\/strong>4 \u5728GaN-26.6\u4e0a\u7684CO<\/strong>2<\/sub><\/strong>\u52a0\u6c22\u7684\u957f\u671f\u7a33\u5b9a\u6027<\/strong>\"\"<\/p>\n

a\uff09\u78b3\u6c22\u5316\u5408\u7269\uff08HCs\uff09\u548c\u542b\u6c27\u5316\u5408\u7269\u7684CO2<\/sub>\u8f6c\u5316\u7387\u548c\u65e0CO\u5206\u5e03\u3002<\/p>\n

b\uff09DME\uff08STYDME\uff09\u7684\u4e0d\u540c\u4ea7\u7269\u7684\u9009\u62e9\u6027\u548c\u65f6\u7a7a\u4ea7\u7387\u3002\u8bef\u5dee\u68d2\u7684\u76f8\u5bf9\u504f\u5dee\u4e3a5\uff05\u3002 \u53cd\u5e94\u6761\u4ef6\uff1aP = 2.0 MPa\uff0cT = 360\u00b0C\uff0cH2<\/sub>\/CO2<\/sub>\u00a0= 2\uff0c\u6c14\u4f53\u6bcf\u5c0f\u65f6\u7a7a\u901f= 3000ml g\u22121<\/sup>\u00a0h\u22121<\/sup>\u3002<\/p>\n

\u56fe<\/strong>5<\/strong>\u00a0\u5728\u4e0d\u540c\u7c92\u5f84\u7684GaN\u50ac\u5316\u5242\u4e0a\uff0cCO\/CO<\/strong>2<\/sub><\/strong>\u52a0\u6c22\u7684\u50ac\u5316\u6027\u80fd<\/strong>\"\"<\/p>\n

\u53cd\u5e94\u6761\u4ef6\uff1aT = 360\u00a0\u00b0C\uff0cP = 2.0 MPa\uff0c\u6c14\u65f6\u7a7a\u901f= 1000 mL g-1<\/sup>\u00a0h–<\/sup>1\u7684CO\u52a0\u6c22\u548c3000 mL g-1<\/sup>\u00a0h-1<\/sup>\u7684CO2<\/sub>\u52a0\u6c22\uff0cH2<\/sub>\/CO\uff08CO2<\/sub>\uff09= 2\uff0c\u84b8\u6c7d\u6301\u7eed\u65f6\u95f4= 40 h\u3002\u8bef\u5dee\u68d2\u7684\u76f8\u5bf9\u504f\u5dee\u57285\uff05\u4ee5\u5185\u3002<\/p>\n

\u56fe<\/strong>6<\/strong>\u00a0\u5b9e\u9a8c\u7ed3\u679c\u8bc1\u5b9eDME\u4e3a\u4e3b\u8981\u4ea7<\/strong>\u7269<\/strong>\"\"<\/p>\n

a\uff09\u63a5\u89e6\u65f6\u95f4\u5bf9360\u00b0C\u4e0bGaN-26.6\u4e0aCO2<\/sub>\u52a0\u6c22\u50ac\u5316\u884c\u4e3a\u7684\u5f71\u54cd\uff08\u63a5\u89e6\u65f6\u95f4\u8868\u793a\u4e3a\u50ac\u5316\u5242\u91cd\u91cf\uff08W\uff09\u9664\u4ee5\u539f\u6599\u6c14\u6d41\u91cf\uff08F\uff09\u3002\u8bef\u5dee\u68d2\u7684\u76f8\u5bf9\u504f\u5dee\u57285\uff05\u4ee5\u5185\uff09\u3002<\/p>\n

b\uff09\u5728P = 2.0 MPa\u548cH2\/CO2<\/sub>= 2 \uff08m\/z\uff1a\u8d28\u8377\u6bd4\uff09\u7684\u6761\u4ef6\u4e0b\uff0cGaN-26.6\u4e0aCO2<\/sub>\u52a0\u6c22\u7684\u7a0b\u5e8f\u5347\u6e29\u8868\u9762\u53cd\u5e94\u66f2\u7ebf\u3002<\/p>\n

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

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