|
||
 | å¡‘æ–™ | Š™¡èƒ¶ | ¾U¤ç»´ | 涂料与æÑaå¢?/a> | 胶粘å‰?/a> | å¤åˆææ–™ | 矛_Œ– | 化工 | 仪器仪表 | æ–îCñ”ä¸?/a> | 专题 | ˜q”回首页 |
|
|
||
| å¡‘æ–™ | Š™¡èƒ¶ | ¾U¤ç»´ | 涂料与æÑaå¢?/a> | 胶粘å‰?/a> | å¤åˆææ–™ | 矛_Œ– | 化工 | 仪器仪表 | æ–îCñ”ä¸?/a> | 专题 | ˜q”回首页 |
|
˜q‘æ—¥åQŒå—京工业大å?/span>固æ€ç¦»å与新能æºæŠ€æœ¯è¯¾é¢˜ç»„利用一¿U有效的两æ¥ç›¸å应法构å¾å‡ºé«˜å¯¼ç”µæ€§ã€é«˜‹zÀL€§çš„å•é’™é’›çŸ¿å‚¬åŒ–剂，探烦了该¿U方法在æå‡é’™é’›çŸ¿åœ¨æ°§æžå‡ºï¼ˆOERåQ‰ä¸Žæ°¢æžå‡ºï¼ˆHERåQ‰æ´»æ€§ä¸çš„作用以åŠç”µè·å†åˆ†å¸ƒå¯¹å‚¬åŒ–活性的影å“ã€?/span>相关æˆæžœä»¥æ ‡é¢˜äØ“â€?/span>Engineering Charge Redistribution within Perovskite Oxides for Synergistically Enhanced Overall Water Splittingâ€?/span>å‘表åœ?/span>ACS Materials Letters。å—京工业大å¦åšå£«ç ”½I¶ç”ŸçŽ‹ä¹ ä¹ äؓ论文½W¬ä¸€ä½œè€…ã€?/span>通讯作者：周呄教授åQŒé‚µå®—åã^教授ã€?/span>
å›?/span>1基础表å¾ã€‚（aåQ‰ä¸¤æ¥ç›¸å应法制备过½E‹ç¤ºæ„图åQ?/span>(b) XRDåQ?/span>(c)SEMåQ?/span>(d) HRTEMå’?/span>(e) å…ƒç´ åˆ†å¸ƒã€?/span>
该工作通过两æ¥ç›¸å应法è”åˆå…ƒç´ 掺æ‚制备得到å•é’™é’›çŸ¿LSFCP-55åQŒå¦‚å›?/span>1a所½Cºï¼Œé¦–å…ˆåˆæˆäº†é’™é’›çŸ¿LSFåQŒç„¶åŽç¬¬äºŒæ¥å¼•å…¥ä¸?/span>LSF一定比例的SCP (SrCO3ã€?/span>Co3O4ã€?/span>NH4H2PO4)。在相å应过½E‹ä¸åQŒè¿™äº›ç¦»å在高温下通过钙钛çŸ?/span>LSF表题q…速扩散到其体相，最¾lˆåÅžæˆé’™é’›çŸ¿LSFCP-55。通过XRDã€?/span>SEMå’?/span>HRTEM表å¾åQŒè¯æ˜Žè¯¥¿U方法得到的钙钛矉K¢—¾_’æ›´ž®ï¼Œòq¶ä¸”所需的煅烧温度更低ã€?/span>æ¤å¤–åQŒé€šè¿‡æ¤ç§æ–ÒŽ³•åˆ¶å¤‡çš?/span>LSFCP-55å…ähœ‰è¾ƒé«˜çš„电导率åQ?/span>94.2 S cm-1åQ‰ï¼Œ˜qœè¿œé«˜äºŽLSFåQ?/span>5.5 S cm-1åQ‰ã€?/span>
å›?/span>2 电化å¦è¡¨å¾ã€‚（aåQ‰æ¯”‹zÀL€§ï¼›åQ?/span>båQ?/span>OERé˜ÀLŠ—图谱åQ›ï¼ˆcåQ?/span>HERé˜ÀLŠ—图谱åQ›ï¼ˆdåQ‰å…¨è§£æ°´è£…ç½®½Cºæ„图；以ä¸åŒå‚¬åŒ–剂作äØ“é˜Ïxžå’Œé˜´æžçš„全解水装¾|®çš„åQ?/span>eåQ‰æžåŒ–曲¾U¿å’ŒåQ?/span>fåQ‰ç¨³å®šæ€§ã€?/span>
利用三电æžä½“¾pÕd¯¹ä¸åŒå‚¬åŒ–剂的OERå’?/span>HER‹zÀL€§è¿›è¡Œæµ‹è¯•ï¼Œå‘现通过两æ¥ç›¸å应法è”åˆå…ƒç´ 掺æ‚制备得到çš?/span>LSFCP-55å…ähœ‰ç›¸å¯¹äº?/span>LSFå’?/span>SCP显著æ高çš?/span>OERå’?/span>HER‹zÀL€§å’Œæœ¬å¾‹zÀL€§ï¼ˆå›?/span>2aåQ‰ã€‚æ¤å¤–，通过½{‰æ•ˆç”µèµ\图拟åˆå¾—到催化剂的电化å¦é˜ÀLŠ—è°?/span>(EIS)。所有催化剂åœ?/span>Nyquist图上都显½CÞZØ“åŠåœ†åQŒåŒ…括电诂{¿UÈ”µé˜?/span>(Rct)ã€æ€ÀL¬§å§†ç”µé˜?/span>(Rs)å’Œæ’相元ä»?/span>(如图2b-c所½C?/span>)。åƈ且，对于OERå’?/span>HERåQ?/span>LSFCP-55å‡æ˜¾½Cºå‡ºæœ€ž®çš„RctåQŒè¿™è¡¨æ˜Žå…¶å应动力å¦æœ€å¿«ï¼Œç”µåä¼ é€’é€Ÿåº¦æœ€å¿«ã€?/span>鉴于LSFCP-55优越的åŒåŠŸèƒ½å‚¬åŒ–‹zÀL€§å’Œ½E›_®šæ€§ï¼Œž®†å…¶åº”用于电解水装置åQŒå¦‚å›?/span>2eåQ?/span>LSFCP-55 ( ) | | LSFCP-55(-)全解水装¾|®åœ¨10mA cm-2的电‹¹å¯†åº¦ä¸‹æ˜„¡¤ºå‡?/span>1.57 V的低电ä½åQŒä½Žäº?/span>RuO2 ( ) | | 20 pt / C (-) (1.60 V)。æ¤å¤?/span>, LSFCP-55 ( ) || LSFCP-55(-)电解水装¾|?/span>å…ähœ‰è¾ƒå¥½çš„æ•´ä½?/span>电解水稳定æ€?/span>åQ?/span>åœ?/span>50 h的时间内昄¡¤ºå‡ø™¾ƒž®çš„电压衰å‡åQ?/span>优于RuO2 ( ) || 20Pt/C(-)ã€?/span>
å›?/span>3 基础表å¾ã€?/span>XPSåQ?/span>(a) Fe 2påQ?/span>(b) Co 2påQ?/span>XPS O 1såQ?/span>(c) LSFåQ?/span>(d) SCPå’?/span>(e) LSFCP-55åQ?/span>(f) LSFåQ?/span>SCPåQ?/span>LSFCP-55å’?/span>LSFCP-Bæ ·å“çš?/span>O2-TPD曲线ã€?/span>
采用 XPSç ”ç©¶å‚¬åŒ–å‰‚çš„ç”µå状æ€ã€?/span>å‘现LSFCP-55相对äº?/span>LSFå’?/span>LSFCP-Bå…ähœ‰è¾ƒé«˜å«é‡çš?/span>Fe4 (16.8 %åQŒå›¾3a)åQŒå…¶å¯ä»¥åŠ 大Fe 3dä¸?/span>O 2pçš„æ‚化程度åÆˆä¸”åŠ é€?/span>OER˜q‡ç¨‹ä¸çš„去质å化速度åQŒå› æ¤å¯ä»¥æé«?/span>OERå’?/span>HER‹zÀL€§ã€‚相对于SCPåQ?/span>LSFCP-55å…ähœ‰è¾ƒä½Žçš?/span>Coä»äh€ï¼ˆå›?/span>3båQ‰ã€‚æ¤å¤–，Co3 / Co4 电å对的å˜åœ¨ä¹Ÿå¯ä»¥æ高催化活性。结å?/span>XPS O1s, LSFCP-55ä¸çš„æ™¶æ ¼æ°§ä½¾|®ç›¸å¯¹äºŽLSFå’?/span>SCPå…ähœ‰æ˜Žæ˜¾çš„æ£å移åQˆå›¾3c-eåQ‰ï¼Œ˜q™ä»£è¡¨éƒ¨åˆ†éž‹zÀL€§æ™¶æ ¼æ°§O2-被催化剂LSFCP-55ä¸çš„强电å相互作用激‹z»ï¼Œè½¬å˜ä¸ºæ´»æ€§æ™¶æ ¼æ°§O2-x。结å?/span>Fe 2p å’?/span>Co 2påQ?/span>LSFCP-55ä¸?/span>FeåQ?/span>Coå’?/span>O¼›Õdçš„ähæ€å˜åŒ–å¯èƒ½æ˜¯ç”׃ºŽ‹zÀL€?/span>Fe和周围原å的强电è·å†åˆ†å¸ƒå¯ÆD‡´çš?/span>åQŒå³é€šè¿‡Fe4 -O2-x-Co3 ˜q›è¡Œäº?/span>大é‡çš„电åè{¿U…R€‚通过˜q™ç§å¼‚常的电è·å†åˆ†é…åQŒä¼˜åŒ–了水的å”R™„和解å¸èƒ½ä»¥åŠä¼˜åŒ–了对äº?/span>OERå应ä¸é—´ç‰©ç§ (M-OHã€?/span>M-OOHå’?/span>M-O)å’?/span>HERå应ä¸é—´‹zÀL€§ç‰©¿U?/span> (H )çš?/span>å”R™„åQŒä»Žè€Œæ高了OERå’?/span>HERçš„æ´»æ€?/span>ã€?/span>O2-TPDåQˆå›¾3fåQ‰å’ŒH2-TPDåQˆå›¾4aåQ?/span>曲线也è¯æ˜Žäº†ä»¥ä¸ŠçŒœæµ‹ã€?/span>
å›?/span>4 基础表å¾ã€?/span>(a) LSFåQ?/span>SCPåQ?/span>LSFCP-55å’?/span>LSFCP-Bæ ·å“çš?/span>H2-TPD曲线åQ?/span>(b) LSFåQ?/span>SCPåQ?/span>(c) LSFCP-55å’?/span>LSFCP-B的接触角åQ?/span>(d)催化剂的拉曼光谱åQ?/span>(e) 催化剂的OER 甉|µå¯†åº¦ä¸?span style="font-family:;">pHçš„å…³¾p»ï¼›(f)æ™¶æ ¼æ°?/span>直接å‚与OERå应åQšåŽŸä½è´¨è°?/span>ã€?/span>
相对äº?/span>LSF(142.7?)ã€?/span>SCP(132.0?)å’?/span>LSFCP(129.9?)åQ?/span>LSFCP-55的接触角(99.2?)较å°åQˆå›¾4b-cåQ?/span>åQ?/span>˜q?/span>è¯å®žäº†é’™é’›çŸ¿ç–水性质的改善，有利于促˜q›æ°´è§£ç¦»ç”Ÿæˆæ°¢å’Œæ°§ã€‚æ¤å¤–，LSFCP-55内部有利的电è·å†åˆ?/span>å¸?/span>å¯èƒ½ä¼šå¢žå¼ºé‡‘属原å和氧原å之间的æ‚化åQŒä»Žè€?/span>æ高HERå’?/span>OER的电åè{¿U?/span>能力(˜q™ä¸ŽEISåQ?/span>RamanåQŒå›¾4d¾l“果一è‡?/span>)。值得注æ„的是åQŒè¿™¿U电å相互作用和高导甉|€§çš„å˜åœ¨ä¹Ÿè¡¨æ˜Žäº†˜q™ç§ä¸¤æ¥åˆ¶å¤‡æ–ÒŽ³•çš„有效性。æ¤å¤–，鉴于部分éžæ´»æ€§æ™¶æ ¼æ°§O2-被催化剂LSFCP-55ä¸çš„强电å相互作用激‹z»ï¼Œè½¬å˜ä¸ºæ´»æ€§æ™¶æ ¼æ°§O2-xåQŒå¯èƒ½æœ‰éƒ¨åˆ†æ™¶æ ¼æ°§å‚ä¸?/span>OERå应。我们首先通过‹¹‹è¯•ä¸åŒpH下的OER性能åQŒåƈ¾l˜åˆ¶ç”‰|µå¯†åº¦ä¸?/span>pHçš„å…³¾pÕd›¾åQŒå‘çŽ?/span>LSFCP-55çš?/span>OER‹zÀL€§æ˜¾½Cºå‡ºè¾ƒå¼ºçš?/span>pHä¾èµ–性（å›?/span>4eåQ‰ã€‚å› æ¤ï¼Œæˆ‘们借助原ä½è´¨è°±˜q›è¡Œ18O‹‚€‹¹‹ä»¥è¯æ˜Žæ™¶æ ¼æ°§å‚与å应的å‘生。如å›?/span>4f所½Cºï¼Œåœ?/span>LSFCP-55催化剂的‹¹‹è¯•˜q‡ç¨‹ä¸ï¼Œè´¨è°±‹‚€‹¹‹åˆ°å¤§é‡34O2 (16O18O)åQŒè¯å®žäº†18Oçš„å˜åœ¨ï¼Œä»¥åŠLSFCP-55ä¸æ›´å¤šçš„æ™¶æ ¼æ°§å‚与了OERå应。相比之下，LSFå’?/span>SCP‹‚€‹¹‹åˆ°çš?/span>34O2å«é‡è¾ƒå°‘åQŒè¡¨æ˜?/span>å…¶ä¸è¾ƒå°‘çš?/span>æ™¶æ ¼æ°§å‚ä¸?/span>OERååº”ã€‚å› æ¤ï¼ŒLSFCP-55ä¸çš„æ™¶æ ¼æ°§è¢«å¼ºç”µè·å†åˆ?/span>å¸?/span>‹È€‹z?/span>åQŒä»Žè€Œå‚与到OERå应˜q‡ç¨‹ä¸ã€?/span>
˜q™é¡¹å·¥ä½œä¸ä»…æ示了电è·å†åˆ†å¸ƒå’Œæ¿€‹zÈš„æ™¶æ ¼æ°§å¯¹æ高电催化活性的作用åQŒè€Œä¸”æ供了一¿U简å•æœ‰æ•ˆçš„制备高活性和高导甉|€§é’™é’›çŸ¿æ°§åŒ–物的æ–ÒŽ³•ã€?/span>
作者简�/strong>
周呄教授åQŒå—京工业大å¦åŒ–å·¥å¦é™¢ï¼Œæ料化å¦å·¥ç¨‹å›½å®¶é‡ç‚¹å®žéªŒå®¤æ•™æŽˆï¼Œåšå£«ç”Ÿå¯¼å¸ˆï¼Œå›½å®¶¾U§é«˜å±‚次引进人æ‰åQŒæ±Ÿè‹ç‰¹è˜æ•™æŽˆï¼Œæ±Ÿè‹çœæ°å‡ºé’òq´åŸºé‡‘获得者，江è‹åŒåˆ›äººæ‰è®¡åˆ’å’ŒåŒåˆ›å›¢é˜Ÿé¢†å†›ähæ‰èŽ·å¾—è€…ã€‚ç ”½I¶æ–¹å‘包括：低温å›ÞZ½“æ°§åŒ–ç‰©ç‡ƒæ–™ç”µæ± å…³é”®æ料；质å交æ¢è†œç‡ƒæ–™ç”µæ± 关键æ料；电解水制氢催化剂。迄今在国际ä¸ÀLµæœŸåˆŠä¸Šå‘è¡?/span>SCI论文300余篇åQŒå¼•ç”?span style="font-family:;">16000余次åQ?/span>h-index=70åQ?/span>å…¶ä¸åŒ…括Natureã€?/span>Nature Energyã€?/span>Nature Communicationsã€?/span>Science Advances½{‰å›½é™…è‘—å刊物ã€?/span>
相关链接
https://pubs.acs.org/doi/10.1021/acsmaterialslett.1c00359
