涓浗鐭蟲(chóng)補(bǔ)澶у錛堝寳浜級(jí)鐜嬮泤鍚涖佹竻鍗庡ぇ瀛︽湵姘告硶銆奀hem. Eng. J.銆? 閫氳繃璋冭妭Pt鐨勫寲瀛︾姸鎬佷績(jī)榪涘厜鍌寲鍒嗚В姘翠駭姘?/span>
2022-05-03 鏉ユ簮:涓浗鑱氬悎鐗╃綉 鐐瑰嚮嬈?/span>
鍏抽敭璇嶏細(xì)鐭沖ⅷ鐩告愛(ài)鍖栫⒊銆丳t0鐗╃銆佸師浣嶇孩澶栥佸厜鍌寲浜ф阿
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?jiǎn)瑙?/span>Pt鍦ㄥ厜鍌寲鍙嶅簲榪囩▼涓殑鐪熷疄鎬ц川錛屽彲浠ヤ負(fù)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(jiǎn)棰樹(shù)負(fù)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?jiǎn)涓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(jiǎn)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(jiǎn)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?jiǎn)楂樻俯鐑仛鍚堛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(ài)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(fù)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(fù)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(fù)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(fù)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(fù)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?shù)?/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(jiǎn)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(fù)浜?jiǎn)姣旇緝锛屾垜浠瑯q樼爺絀朵簡(jiǎn)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(jiǎn)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(jiǎn)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?shù)?/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(fù)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(jiǎn)榪涗竴姝ョ爺絀?/span>Pt鐗╃鐨勫獎(jiǎng)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?jiǎn)涓嶅悓缁撴瀯妯″瀷瀵瑰簲鐨?/span>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(jiǎn)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(shù)簡(jiǎn)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(fù)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(jiǎn)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(jiǎn)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?shù)?/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(jiǎn)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(fù)涓浗鐭蟲(chóng)補(bǔ)澶у錛堝寳浜級(jí)鍗氬＋鐢熸浣蟲(chóng)槦錛岃鏂囬氳浣滆呬負(fù)涓浗鐭蟲(chóng)補(bǔ)澶у錛堝寳浜級(jí)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
鍏嶈矗澹版槑錛氶儴鍒嗚祫鏂欐潵婧愪簬緗戠粶錛岃漿杞界殑鐩殑鍦ㄤ簬浼犻掓洿澶氫俊鎭強(qiáng)鍒嗕韓錛屽茍涓嶆剰鍛崇潃璧炲悓鍏惰鐐規(guī)垨璇佸疄鍏剁湡瀹炴э紝
涔熶笉鏋勬垚鍏朵粬寤鴻銆備粎鎻愪緵浜ゆ祦騫沖彴錛屼笉涓哄叾鐗堟潈璐熻矗銆傚娑夊強(qiáng)渚墊潈錛岃鑱旂郴鎴戜滑鍙?qiáng)鏃朵慨鏀规垨鍒犻櫎銆?br>閭錛歩nfo@polymer.cn
錛堣矗浠葷紪杈戯細(xì)sun錛?
- 鐩稿叧鏂伴椈
- 鏃犵浉鍏蟲(chóng)柊闂?/li>
