銆銆4鏈?3鏃ワ紝涓闄㈠ぇ榪炲寲鐗╂墍鍌寲鍩虹鍥藉閲嶇偣瀹為獙瀹ら珮鏁﹀嘲銆佹豹鍥介泟鍜屽寘淇″拰闄㈠＋絳夌爺絀朵漢鍛樹笌嫻欐睙宸ヤ笟澶у鐜嬪緩鍥芥暀鎺堢瓑鍚堜綔錛屽湪浜屾哀鍖栫⒊楂樻晥鐢?shù)鍌寲杩樺師鐮斀I朵腑鍙栧緱榪涘睍錛屽彂鐜扮撼綾抽挴鐢墊瀬楂樻晥鍌寲浜屾哀鍖栫⒊榪樺師鐢熸垚涓姘у寲紕籌紝騫朵笖鍏跺偓鍖栨ц兘涓庣撼綾崇矑瀛愬昂瀵告湁寰堝己鐨勪緷璧栧叧緋匯傜浉鍏崇粨鏋滃彂琛ㄥ湪鏃ュ墠鍑虹増鐨勩婄編鍥藉寲瀛︿細蹇椼?J. Am. Chem. Soc. 2015, 137, 4288鈭?291)涓娿?
銆銆榪戝勾鏉ワ紝鍏ㄧ悆浜屾哀鍖栫⒊鎺掓斁閲忕殑閫愬勾澧炲姞瀵逛漢浠禆浠ョ敓瀛樼殑鐢熸佺幆澧冮犳垚浜嗕弗閲嶅▉鑳侊紝鍥犳浜屾哀鍖栫⒊鐨勬崟鑾楓佸瓨鍌ㄤ互鍙婅漿鍖栧彈鍒扮爺絀惰呯殑騫挎硾鍏蟲敞銆傚湪浜屾哀鍖栫⒊杞寲鏂歸潰錛屽埄鐢ㄤ紶緇熷寲瀛︽柟娉曡繕鍘熶簩姘у寲紕抽渶瑕佸悓鏃舵彁渚涜兘閲忓拰姘㈡皵錛岃岄噰鐢ㄧ數(shù)鍌寲鏂規(guī)硶榪樺師浜屾哀鍖栫⒊錛屼笌鐢?shù)瑙ｆ按鑰﹀悎浠庢按涓幏鍙栨阿錛屽彲浠ュ湪姣旇緝娓╁拰鐨勫弽搴旀潯浠朵竴姝ョ洿鎺ヨ幏寰椾竴姘у寲紕熾佺⒊姘㈠寲鍚堢墿鍜岀敳閱囩瓑楂樺煎寲瀛﹀搧鍜屾恫浣撶噧鏂欍傚悓鏃訛紝璇ヨ繃紼嬩笌鍙啀鐢熻兘婧愭垨瀵屼綑鏍歌兘鍒╃敤鐩哥粨鍚堬紝瀹炵幇澶ц妯＄數(shù)鑳藉瓨鍌紝琛ㄧ幇鍑烘瀬鍏鋒綔鍔涚殑搴旂敤鍓嶆櫙錛屽綋鍓嶅凡鎴愪負鐩稿叧棰嗗煙涓涓噸瑕佺殑鐮旂┒鐑偣銆?
銆銆Pd鏄吀鍨嬬殑鏋愭阿鍙嶅簲鍌寲鍓傦紝浣撶浉Pd鐢墊瀬涓婄殑CO2榪樺師榪囩數(shù)鍔塊珮銆佺珵浜夋х殑鏋愭阿鍙嶅簲閫犳垚娉曟媺絎晥鐜囦綆銆傝鍥㈤槦鐨勫疄楠岀爺絀跺彂鐜幫紝鍦?.4鈥?0.3 nm鑼冨洿鍐咃紝Pd綰崇背綺掑瓙鐨凜O2榪樺師閫夋嫨鎬у拰媧繪ц〃鐜頒簡鏄庢樉鐨勫昂瀵鎬緷璧栨с傚湪鈭?.89 V (vs. RHE)鏃剁敓鎴怌O鐨勬硶鎷夌鏁堢巼浠?0.3 nm Pd涓婄殑5.8%澧炲姞鍒?.7 nm Pd涓婄殑91.2%錛屽悓鏃剁敓鎴怌O鐨勭數(shù)嫻佸瘑搴﹀鍔犱簡18.4鍊嶃傞氳繃瀵嗗害娉涘嚱鐞嗚(DFT)璁＄畻錛屽垎鏋愪簡鍦ㄤ笁縐嶄笉鍚屽弽搴斾綅(騫抽潰銆佸彴闃跺拰瑙掍綅)涓奀O2榪樺師鍜屾瀽姘㈠弽搴旂殑鑷敱鑳斤紝騫跺緩绔嬩簡鍙嶅簲鎬ц兘涓庣矑搴︾殑鍏崇郴銆傜敓鎴怌O鐨勮漿鎹㈤鐜?TOF)涓庣矑寰勫憟鐜扮伀灞卞瀷鏇茬嚎鍏崇郴錛岃繖琛ㄦ槑鍙互閫氳繃鏀瑰彉Pd綰崇背綺掑瓙鐨勫昂瀵告潵璋冨彉CO2鍚擱檮銆佷腑闂寸墿縐岰OOH*鐨勫艦鎴愪互鍙奀O*鐨勮劚闄勭瓑錛屼粠鑰屽疄鐜癙d綰崇背綺掑瓙浠庢瀽姘㈠偓鍖栧墏鍒伴珮鏁圕O2榪樺師鍌寲鍓傜殑杞彉銆?
銆銆璇ョ爺絀跺緱鍒頒簡鍥藉鑷劧縐戝鍩洪噾濮斿拰縐戞妧閮ㄧ瓑鐩稿叧欏圭洰鐨勮祫鍔┿?
