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鍖栧伐
褰撳墠浣嶇疆錛?棣栭〉 >> 璧勮 >> 鍖栧伐 >> 琛屼笟鍔ㄦ?/a> >> 姝ｆ枃

  璐甸噾灞?span style="font-family:;">Pt鍥犲叾鍏鋒湁鍚堥傜殑璐圭背鑳界駭鑰岃鐢ㄤ綔甯哥敤鐨勫姪鍌寲鍓傦紝鍏鋒湁媧繪ч珮銆佺ǔ瀹氭уソ絳変紭鍔褲備綔涓哄姪鍌寲鍓傦紝Pt鐨勫寲瀛︾姸鎬佸鍏夊偓鍖栧墏鐨勬瀽姘㈡椿鎬ф湁鏄捐憲褰卞搷錛屼絾榪欑褰卞搷灝氭湭寰楀埌娣卞叆鐮旂┒銆傛洿涓洪噸瑕佺殑鏄紝浜嗚ВPt鍦ㄥ厜鍌寲鍙嶅簲榪囩▼涓殑鐪熷疄鎬ц川錛屽彲浠ヤ負鏋勫緩鍏鋒湁楂樻椿鎬х殑鍏夊偓鍖栧墏鎻愪緵鏂扮殑鎬濊礬銆?/span> 榪戞湡錛屼腑鍥界煶娌瑰ぇ瀛︼紙鍖椾含錛夌帇闆呭悰鍓爺絀跺憳璇鵑緇勪笌娓呭崕澶у鏈辨案娉曟暀鎺堝湪銆?/span>Chemical Engineering Journal銆?/span>鏈熷垔涓婂彂琛ㄤ簡棰樹負鈥?/span>Boosting photocatalytic hydrogen evolution via regulating Pt chemical states鈥濈殑鏂囩珷錛?span style="font-family:;">DOI錛?/span>10.1016/j.cej.2022.136334錛夈傛湰璁烘枃鎻愬嚭浜嗕竴縐嶆湁鏁堢殑絳栫暐錛岄氳繃璋冭妭Pt鐨勫寲瀛︾姸鎬佹潵澶у箙搴︽彁楂?/span>Pt/g-C3N4鍏夊偓鍖栧墏鐨勪駭姘㈡ц兘銆傛枃涓埗澶囦簡涓嶅悓Pt0鍚噺鐨?/span>Pt/g-C3N4鍌寲鍓傦紝鍙戠幇鎻愰珮Pt0鍚噺鍙互澶у箙鎻愰珮鍏夎В姘翠駭姘㈡椿鎬с傚師浣嶇孩澶栧厜璋卞拰DFT鐞嗚璁＄畻璇佹槑錛屾皵姘?/span>澶勭悊浣跨數(shù)瀛愪粠g-C3N4鐨?/span>N鍘熷瓙杞Щ鍒?/span>Pt2 涓?/span>錛屼粠鑰屽鍔犱簡Pt0鐗╃鐨勬暟閲忋?/span>Pt0鐗╃鐨勫ぇ閲忕敓鎴愭湁鍒╀簬鍔犻熷厜鐢熺數(shù)鑽風(fēng)殑鍒嗙銆傛澶栵紝Pt0姣?/span>Pt2 鍏鋒湁鏇翠綆鐨勬阿姘斿惛闄勮兘錛屾湁鍒╀簬姘㈡皵鐨勬孩鍑恒傚洜姝わ紝鍏鋒湁楂樻瘮渚?/span>Pt0鐨勫厜鍌寲鍓傚叿鏈夋洿楂樼殑浜ф阿媧繪с?/span>


  鏈枃閲囩敤浜嗛珮娓╃儹鑱氬悎銆佽秴澹版箍嫻告笉錛?/span>1.0%-Pt/CN錛夈佸厜娌夌Н錛?/span>1.0%-Pt/CN-P錛夈?/span>NaBH4娑茬浉榪樺師錛?/span>1.0%-Pt/CN-BH錛夊拰姘㈡愛娣峰悎姘旂儹澶勭悊錛?/span>1.0%-Pt/CN-BH-H錛夌瓑鏂規(guī)硶鍒跺浜?/span>Pt/g-C3N4澶嶅悎鏉愭枡銆傞氳繃XPS琛ㄥ緛鍙戠幇Pt涓昏浠?/span>Pt0鐗╃鐨勫艦寮忓瓨鍦ㄤ簬1.0%-Pt/CN-BH-H鏍峰搧涓傜浉鍙嶏紝Pt涓昏浠?/span>Pt2 褰㈠紡瀛樺湪浜?/span>1.0%-Pt/CN-P鍜?/span>1.0%-Pt/CN-BH鏍峰搧涓傜粡榪囨阿姘販鍚堟皵姘涘鐞嗗悗錛?/span>Pt鐨勫寲瀛︾姸鎬佸彂鐢熸樉钁楀彉鍖栵紝1.0%-Pt/CN-BH-H涓?/span>Pt0鐨勬瘮渚嬫樉钁楀鍔犮?/span>1.0%-Pt/CN-P, 1.0%-Pt/CN-BH鍜?1.0%-Pt/CN-BH-H涓?/span>Pt0鐨勬瘮渚嬪垎鍒負8.2%錛?/span>10.0%鍜?/span>60.1%錛堝浘1c錛夈傜粡榪囨皵姘涘鐞嗗悗錛?/span>N鍏冪礌鍚戦珮緇撳悎鑳芥柟鍚戠Щ鍔紝Pt鍏冪礌鍚戜綆緇撳悎鑳芥柟鍚戠Щ鍔紝琛ㄦ槑鐢?shù)瀛愪?/span>N鍚?/span>Pt0杞Щ錛堝浘1b錛?/span>銆傝繖浜涚粨鏋滆〃鏄庯紝1.0%-Pt/CN-BH-H涓惈鏈夊ぇ閲忕殑Pt0鐗╃鏈夊埄浜庣數(shù)鑽風(fēng)殑鍒嗙鍜岃漿縐匯?/span>閫氳繃CO鍚擱檮綰㈠鍏夎氨錛堝浘1d錛夊緱鍑?/span>2115 cm-1澶勭殑鍚擱檮宄?/span>涓?/span>CO鍦?/span>Pt2 鐗╃涓婄殑鍚擱檮銆?/span>2055 cm-1澶勭殑鍚擱檮宄?/span>涓?/span>CO鍦?/span>Pt0鐗╃涓婄殑綰挎у惛闄勩?/span>緇忚繃姘旀皼澶勭悊鍚庯紝Pt0鐗╃鐨勬瘮渚嬫樉钁楀鍔犮傝繖涓緇撹涓?/span>XPS緇撴灉淇濇寔涓鑷?/span>銆?/span>


鍥?/span>1 錛?/span>a錛?/span>XPS鍏ㄨ氨銆?/span>鏍峰搧鐨?/span>N 1s錛?/span>b錛夊拰Pt 4f錛?/span>c錛夊厓绱犺氨銆?/span>錛?/span>d錛夋牱鍝佺殑CO鍚擱檮綰㈠鍏夎氨銆?/span>

   鍦ㄥ彲瑙佸厜鏉′歡涓嬶紝1.0 %-Pt/CN-BH-H 鏍峰搧錛?/span>Pt0鐨勬瘮渚嬩負60.1%錛?/span>鍏鋒湁鏈楂樼殑鍏夊偓鍖栨椿鎬?/span>錛?/span>2.316 mmol h-1 g-1錛?/span>錛岀害涓?/span>1.0 %-Pt/CN-P 鏍峰搧錛?/span>0.605 mmol h-1 g-1 , Pt0鐨勬瘮渚嬩負8.2%錛?/span>鍜?/span>1.0%-Pt/CN-BH鏍峰搧錛?/span>0.644 mmol h-1 g-1 , Pt0鐨勬瘮渚嬩負10.0%錛?/span>鐨?/span>4鍊?/span>錛堝浘2a錛?/span>銆傚洜姝わ紝鍌寲媧繪т笌Pt鐗╃鐨勫寲瀛︾姸鎬佹湁鍏熾?/span>鎴戜滑鍙互璁や負錛?/span>1.0%-Pt/CN-BH-H涓?/span>Pt0鐨勬瘮渚?/span>瓚婇珮錛屽厜鍌寲鎬ц兘瓚婂ソ銆傞氳繃澶氭寰幆瀹為獙琛ㄦ槑1.0%-Pt/CN-BH-H鍏鋒湁浼樺紓鐨勭ǔ瀹氭?/span>錛堝浘2b錛夈?/span>1.0%-Pt/CN-BH-H鍦?/span>420 nm涓嬬殑琛ㄨ閲忓瓙鏁堢巼涓?/span>8.1%錛屾樉钁楅珮浜?/span>1.0%-Pt/CN-P錛?/span>4.0%錛?/span>錛岃鏄庡墠鑰呭湪鍙鍏夋潯浠朵笅鍏鋒湁浼樿秺鐨勬椿鎬?/span>錛堝浘2c錛?/span>銆?/span>


鍥?/span>2 媧繪ф祴璇曘傦紙a錛夋牱鍝佸湪鍙鍏夛紙位 鈮?420 nm錛変笅鐨勫厜鍌寲浜ф阿閫熺巼銆傦紙b錛?/span>1.0%-Pt/CN- BH-H鐨勫厜鍌寲浜ф阿寰幆瀹為獙銆傦紙c錛?/span>1.0%-Pt/CN-P鍜?/span>1.0%-Pt/CN-BH-H鍦?/span>420鍜?/span>450 nm澶勭殑鍗曟嘗闀胯〃瑙傞噺瀛愭晥鐜囥?/span>錛?/span>d錛変笉鍚?/span>Pt/g-C3N4澶嶅悎鏉愭枡鍏夊偓鍖栦駭姘㈤熺巼鐨勬瘮杈冦?/span>


  涓轟簡鐮旂┒涓嶅悓Pt鐗╃錛?/span>Pt2 鍜?/span>Pt0錛?/span>涓?/span>g-C3N4涔嬮棿鐨勭數(shù)鑽峰垎紱繪晥鐜囷紝鎴戜滑嫻嬮噺浜?/span>1.0%-Pt/CN-BH-H鍜?/span>1.0%-Pt/CN-P鍦ㄥ彲瑙佸厜鏉′歡涓嬬殑鍘熶綅綰㈠鍏夎氨銆?/span>涓?/span>1.0%-Pt/CN-BH-H鍦ㄩ粦鏆楁潯浠朵笅鐩稿杈冧綆鐨?/span>宄?/span>寮虹浉姣旓紝闅忕潃鍏夌収鏃墮棿鐨勫鍔狅紝鐗瑰緛宄版樉钁楁彁楂?/span>錛?/span>鍥?/span>3a錛?/span>銆?/span>822 cm-1澶勭殑宄板綊鍥犱簬涓冨棯鐜殑浼哥緝鎸姩錛?/span>886 cm-1澶勭殑宄板綊鍥犱簬N-H閿殑寮洸鎸姩銆?/span>鍦?/span>1489鍜?/span>1710 cm-1闄勮繎鐨勫嘲鍒嗗埆瀵瑰簲浜庢潅鐜腑鐨?/span>-C=N鍜?/span>N-C=N錛岃屽湪1338 cm-1闄勮繎鐨勫嘲鍒欐潵婧愪簬-CN鐨勪幾緙┿傞殢鐫鍏夌収鏃墮棿鐨勫鍔狅紝宄?/span>鐨?/span>寮哄害鏄庢樉澧炲ぇ錛屽嘲浣嶇疆淇濇寔涓嶅彉銆傝繖浜涚粨鏋滆〃鏄庯紝1.0%-Pt/CN-BH-H鏍峰搧涓?/span>g-C3N4鐨勭粨鏋勫拰鍖栧閿湪鍙鍏?/span>鐓у皠涓嬬敱浜庡己鐑堢殑鐢?shù)瀛愪紶閫掕屽彂鐢熸槑鏄懼彉鍖?/span>銆備負浜嗘瘮杈冿紝鎴戜滑榪樼爺絀朵簡1.0%-Pt/CN-P鏍峰搧錛?/span>鍥?/span>3b錛?/span>銆?/span>1.0%-Pt/CN-P娌℃湁鏄庢樉鐨勫嘲鐨?/span>鍙?/span>鍖?/span>錛岃繖鍙兘鏄敱浜?/span>Pt2 涓?/span>g-C3N4涔嬮棿鐨勭數(shù)瀛愯漿縐昏兘鍔涜緝宸墍鑷淬傝繖浜涚粨鏋滆〃鏄庯紝楂?/span>Pt0姣斾緥鏈夊埄浜庣數(shù)鑽風(fēng)殑鍒嗙鍜屼駭姘㈡椿鎬х殑鎻愰珮銆?/span>


  涓轟簡鎻ず1.0%-Pt/CN-BH-H涓?/span>Pt0鐨勫艦鎴愭満鐞嗭紝閲囩敤鍘熶綅綰㈠鍏夎氨妯℃嫙浜?/span>1.0%-Pt/CN-BH鐨勬阿姘販鍚?/span>姘旀皼澶勭悊榪囩▼銆傚鍥?/span>3c鍜?/span>3d鎵紺猴紝C-N鏉傜幆涓?/span>C-N閿殑宄板湪1200-1750 cm-1鑼冨洿鍐呮樉钁楀鍔犮傞殢鐫鐒欑儳娓╁害鐨勫崌楂橈紝C-N閿殑鎸姩妯″紡鍙戠敓鏀瑰彉錛?/span>1710 cm-1澶勭殑宄板己搴﹂愭笎澧炲己錛岃〃鏄?/span>C3N4緇撴瀯涓?/span>N鍏冪礌鐨勭數(shù)璐熸у彂鐢熸敼鍙?/span>錛?/span>鍥?/span>3d錛?/span>銆傝繖浜涚粨鏋滆瘉瀹炰簡鍦ㄦ皵姘?/span>澶勭悊榪囩▼涓紝褰撶數(shù)瀛愪粠N鍏冪礌杞Щ鍒?/span>Pt鏃訛紝澶ч噺鐨?/span>Pt2 杞彉涓?/span>Pt0鐗╃銆?/span>鍥犳錛屾垜浠彲浠ユ帹鏂?/span>1710 cm-1澶勫嘲寮?/span>鐨勫彉鍖栨槸鐢變簬C-N閿?/span>閿兘鐨勫彉鍖栵紝琛ㄦ槑g-C3N4緇撴瀯涓?/span>N鍏冪礌鐢?shù)璐熸х殑鍙樺寲銆傝繖浜涚粨鏋滆瘉瀹?/span>鍦?/span>姘旀皼鐒欑儳榪囩▼涓紝澶ч噺鐨?/span>Pt2 閫氳繃N鍏冪礌鐨勫惛寮曠數(shù)瀛愯漿鍖栦負Pt0鐗╃銆?/span>


鍥?/span>3 鍘熶綅綰㈠琛ㄥ緛銆?/span>錛?/span>a錛?/span>1.0%-Pt/CN-BH-H鍜岋紙b錛?/span>1.0%-Pt/CN-P鍦ㄥ彲瑙佸厜錛?/span>位 鈮?420 nm錛?/span>鐓у皠涓嬬殑鍘熶綅綰㈠鍏夎氨銆?/span>錛?/span>c錛?/span>1.0%-Pt/CN-BH鍦ㄦ皵姘涘鐞?/span>鍜屽姞鐑?/span>榪囩▼涓殑鍘熶綅綰㈠鍏夎氨鍜?/span>錛?/span>d錛?/span>灞閮ㄦ斁澶у浘銆?/span>


  涓轟簡榪涗竴姝ョ爺絀?/span>Pt鐗╃鐨勫獎鍝嶏紝鎴戜滑寤虹珛浜?/span>Pt涓?/span>g-C3N4錛?/span>鍥?/span> 4a鍜?4d錛?/span>涔嬮棿鐨勪紭鍖栫粨鏋勬ā鍨嬨傝妯″瀷浠ｈ〃浜嗕笉鍚岀粨鏋勬ā鍨嬪搴旂殑Pt鐨勪笉鍚岄厤浣嶆ā寮忓拰鐘舵侊紝鍖呮嫭Pt2 鍜?/span>Pt0鐗╃銆傜數(shù)鑽峰瘑搴﹀樊鍥炬樉紺轟簡鐢?shù)瀛愬瘑搴︾殑澶畯锛屽鍥?/span>4b鍜?/span>4e鎵紺恒傛牴鎹?/span>Bader鐢?shù)鑽峰垎鏋愬Q屽湪Pt2 鐗╃瀛樺湪涓嬶紝鐢?shù)瀛愪?/span>Pt鍚?/span>g-C3N4杞Щ錛岃漿縐婚噺涓?/span>1.24銆傚綋瀛樺湪Pt0鐗╃鏃訛紝鐢?shù)瀛愪?/span>g-C3N4杞Щ鍒?/span>Pt錛岃漿縐婚噺涓?/span>0.68銆傝繖浜涚粨鏋滆〃鏄庯紝Pt2 鐗╃鐨勫瓨鍦ㄤ笉鍒╀簬鐢?shù)瀛愮殑鎹曡帡鱻?/span>鍦?/span>1.0%-Pt/CN-BH-H鏍峰搧涓?/span>錛?/span>鐢變簬Pt0鐗╃姣斾緥杈冮珮錛屼笖Pt0鐨?/span>鐢?/span>鎴愭彁楂樹簡鐢?shù)鑽峰垎绂绘晥鐜囧Q?/span>g-C3N4涓婄殑鐢?shù)瀛愭洿楂樻晥鍦拌浆绉诲?/span>Pt涓娿?/span>Pt鍦ㄤ笉鍚屽寲瀛︾姸鎬佷笅瀵規(guī)阿姘旂殑鍚擱檮鑳藉鍥?/span>4c鍜?/span>4f鎵紺恒?/span>閫氳繃璁＄畻寰楀埌Pt2 鍜?/span>Pt0鐨勫惛闄勮兘鍒嗗埆涓?/span>-0.105鍜?/span>-0.098 eV銆?/span>Pt2 鍜?/span>Pt0鐨勫惛闄勮窛紱誨垎鍒負2.63鍜?/span>2.79 ?銆傜敱浜?/span>Pt0鐗╃鍏鋒湁杈冧綆鐨勫惛闄勮兘錛屽湪鍚湁Pt0鐗╃鐨勫偓鍖栧墏涓紝姘?/span>姘?/span>鏇村鏄撴孩鍑恒傚洜姝わ紝鎴戜滑鍙互寰楀嚭澧炲姞Pt0鐗╃鍚噺鏈夊埄浜庢瀽姘€傝繖涓緇撴灉涔熶笌涓婅堪鍘熶綅綰㈠鍏夎氨鐨勭粨璁轟竴鑷淬傛澶栵紝榪樿鏄庝簡Pt0鐗╃鍦ㄥ厜鍌寲鍒舵阿涓殑浼樿秺鎬с?/span>


鍥?/span>4 DFT鐞嗚璁＄畻銆傦紙a錛?/span>d錛?/span>浼樺寲緇撴瀯錛?/span>錛?/span>b錛?/span>e錛?/span>宸?/span>鍒?/span>鐢?shù)鑽峰瘑搴﹀?/span>錛?/span>c錛?/span>f錛?/span>Pt2 鍜?/span>Pt0鐗╃瀵規(guī)阿姘?/span>鐨勫惛闄勮兘銆?/span>


  鏈爺絀舵垚鍔熷埗澶囦簡楂?/span>Pt0姣斾緥錛?/span>60.1%錛?/span>鐨勫厜鍌寲鍓傘?/span>瀹冪殑鍏夊偓鍖栦駭姘㈤熺巼杈懼埌2.316 mmol h-1 g-1錛屾瘮鍙鍏夌収灝?/span>錛?/span>位 鈮?420 nm錛?/span>涓?/span>Pt0姣斾緥杈冧綆錛?/span>8.2%錛?/span>鐨?/span>1.0%-Pt/CN-P錛?/span>0.605 mmol h-1 g-1錛?/span>鎻愰珮浜?/span>4鍊嶃?/span>1.0%-Pt/CN-BH-H鐨勯珮鍏夊偓鍖栨ц兘鍙綊鍥犱簬鍏朵腑鍚湁澶ч噺鐨?/span>Pt0鐗╃錛屽姞閫熶簡鍏夌敓鐢?shù)鑽风殑鍒喖?/span>銆?/span>鍙﹀錛?/span>Pt0鐗╃杈冧綆鐨勫惛闄勮兘鏈夊埄浜庢阿姘旂殑婧㈠嚭銆傚洜姝わ紝璋冩帶鍖栧鐘舵佸彲鑳芥槸寮鍙戞柊鍨嬪厜鍌寲鍓傜殑鏈夋晥絳栫暐銆?/span>


璁烘枃絎竴浣滆呬負涓浗鐭蟲補澶у錛堝寳浜級鍗氬＋鐢熸浣蟲槦錛岃鏂囬氳浣滆呬負涓浗鐭蟲補澶у錛堝寳浜級鐜嬮泤鍚涘壇鐮旂┒鍛樺拰娓呭崕澶у鏈辨案娉曟暀鎺堛傛鐮旂┒寰楀埌鍥藉閲嶇偣鐮斿彂璁″垝絳夎祫鍔╂敮鎸併?/span>


鍘熸枃閾炬帴

https://www.sciencedirect.com/science/article/pii/S1385894722018290

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