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1.国能国源电力(北京)有限公司,北京 100033
2.太原理工大学 安全与应急管理工程学院,山西 太原 030024
3.山西鲁能河曲电煤开发有限责任公司 上榆泉煤矿,山西 忻州 036500
4.国源电力(神东电力)公司 技术支持中心,陕西 西安 710000
5.山西省国有资本运营有限公司,山西 太原 030006
Received:23 December 2025,
Revised:2026-04-01,
Online First:16 June 2026,
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刘赛,王晓波,张云峰等.n(Pd)/n(Pt)对Pd-Pt/Al2O3催化甲烷燃烧性能的影响[J].低碳化学与化工,DOI:10.12434/j.issn.2097-2547.20250488.
LIU Sai,WANG Xiaobo,ZHANG Yunfeng,et al.Effects of n(Pd)/n(Pt) on performances of Pd-Pt/Al2O3 catalysts for methane catalytic combustion[J].Low-Carbon Chemistry and Chemical Engineering,DOI:10.12434/j.issn.2097-2547.20250488.
刘赛,王晓波,张云峰等.n(Pd)/n(Pt)对Pd-Pt/Al2O3催化甲烷燃烧性能的影响[J].低碳化学与化工,DOI:10.12434/j.issn.2097-2547.20250488. DOI:
LIU Sai,WANG Xiaobo,ZHANG Yunfeng,et al.Effects of n(Pd)/n(Pt) on performances of Pd-Pt/Al2O3 catalysts for methane catalytic combustion[J].Low-Carbon Chemistry and Chemical Engineering,DOI:10.12434/j.issn.2097-2547.20250488. DOI:
甲烷催化燃烧反应是控制甲烷排放的重要方法。然而,Pd基催化剂在反应工况下存在的烧结失活问题制约了其工业化应用,开发兼具高催化活性和优异抗烧结性能的催化剂是该领域的关键挑战。为阐明Pd-Pt双金属催化剂中
n
(Pd)/
n
(Pt)对活性物种尺寸和催化剂催化性能的影响规律,在固定Pd和Pt总负载量(质量分数)为0.46%的条件下,采用浸渍法制备了不同
n
(Pd)/
n
(Pt)的Pd-Pt/Al
2
O
3
双金属催化剂,并通过XRD和N
2
吸/脱附等表征方法研究了催化剂的物化性质。在固定床反应器上研究了催化剂的催化甲烷燃烧性能。结果表明,在
n
(Pd)/
n
(Pt) = 12.2的Pd-Pt/Al
2
O
3
双金属催化剂(Pd-Pt/Al
2
O
3
(12.2))中,Pd/Pt物种为尺寸0.5~2.0 nm的亚纳米团簇,且Pd/Pt物种通过氧桥键优先落位于五配位AlO
5
位点上。Pd-Pt/Al
2
O
3
(12.2)兼具良好的催化活性和稳定性,其
T
50
(甲烷转化率达到50%时的反应温度)和失活速率分别为396 ℃和0.0082%/h。
Methane catalytic combustion is a key method for controlling methane emissions. However
the deactivation of Pd-based catalysts due to sintering under reaction conditions limits their industrial application
and the development of catalysts that combine high catalytic activities with excellent anti-sintering properties is a key challenge in the field. To elucidate the effects of
n
(Pd)/
n
(Pt) on the sizes of active species and the catalytic performances of Pd-Pt bimetallic catalysts
Pd-Pt/Al
2
O
3
bimetallic catalysts with varying
n
(Pd)/
n
(Pt) were prepared by impregnation method
whilst keeping the total loading amount (mass fraction) of Pd and Pt at 0.46%. The physicochemical properties of the catalysts were investigated by characterization methods such as XRD and N
2
adsorption/desorption. The performances of the catalysts for methane catalytic combustion were investigated in a fixed-bed reactor. The results indicate that in the Pd-Pt/Al
2
O
3
bimetallic catalyst with
n
(Pd)/
n
(Pt) = 12.2 (Pd-Pt/Al
2
O
3
(12.2))
the Pd/Pt species consist of sub-nanometre clusters ranging in size from 0.5 nm to 2.0 nm
and the Pd/Pt species are preferentially located at pentacoordinate AlO
5
sites via oxygen-bridge bonds. Pd-Pt/Al
2
O
3
(12.2) exhibits both good catalytic activity and stability
with
T
50
(the reaction temperature at which the methane conversion rate reaches 50%) of 396 °C and deactivation rate of 0.0082%/h.
YU X , GENZ N S , MENDES R G , et al . Anchoring PdO x clusters on defective alumina for improved catalytic methane oxidation [J ] . Nature Communications , 2024 , 15 : 6494 .
ZHANG C L , CHEN X Y , ZHANG X Y , et al . Advances in the influencing factors and reaction mechanisms of Pd-based supported catalysts for catalytic methane combustion [J ] . Journal of Materials Chemistry A , 2025 , 13 ( 22 ): 16382 - 16413 .
RYU S H , KIM S , LEE H , et al . Robust palladium oxide nano-cluster catalysts using atomic ions and strong interactions for high-performance methane oxidation [J ] . Nature Communications , 2024 , 15 : 8348 .
YANG X W , LI Q , LU E J , et al . Taming the stability of Pd active phases through a compartmentalizing strategy toward nanostructured catalyst supports [J ] . Nature Communications , 2019 , 10 : 1611 .
FENG X B , JIANG L , LI D Y , et al . Progress and key challenges in catalytic combution of lean methane [J ] . Journal of Energy Chemistry , 2022 , 75 : 173 - 215 .
DUAN H M , KONG F X , BI X Z , et al . Catalytic combustion of methane over noble metal catalysts [J ] . ACS Catalysis , 2024 , 14 ( 23 ): 17972 - 17992 .
WANG C , XU Y X , TANG J W . Catalytic methane removal to mitigate its environmental effect [J ] . Science China Chemistry , 2023 , 66 : 1032 - 1051 .
HUANG X , ZHANG X Q , DENG C B , et al . Boosting methane catalytic combustion by confining PdO-Pd interfaces in zeolite nanosheets [J ] . Fuel , 2023 , 344 : 127693 .
黄鑫 , 焦熙 , 黄国宝 , 等 . 甲烷催化燃烧钯基催化剂研究进展 [J ] . 低碳化学与化工 , 2023 , 48 ( 5 ): 147 - 154 .
HUANG X , JIAO X , HUANG G B , et al . Research progress on Pd-based catalysts for methane catalytic combustion [J ] . Low-Carbon Chemistry and Chemical Engineering , 2023 , 48 ( 5 ): 147 - 154 .
张洪雁 , 杜双利 , 王雪峰 . 非贵金属氧化物甲烷催化燃烧催化剂的研究进展 [J ] . 天然气化工—C1化学与化工 , 2021 , 46 ( 2 ): 10 - 14 .
ZHANG H Y , DU S L , WANG X F . Research progress of non-noble metal catalysts for methane catalytic combustion [J ] . Natural Gas Chemical Indutry , 2021 , 46 ( 2 ): 10 - 14 .
LI TENG , BECK A , KRUMEICH F , et al . Stable palladium oxide clusters encapsulated in Silicalite-1 for complete methane oxidation [J ] . ACS Catalysis , 2021 , 11 ( 12 ): 7371 - 7382 .
YANG J Y , HUANG Y K , QI H F , et al . Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration [J ] . Nature Communication , 2022 , 13 : 4244 .
LIU Z , XU G Y , ZENG L Y , et al . Anchoring Pt-doped PdO nanoparticles on γ -Al 2 O 3 with highly dispersed La sites to create a methane oxidation catalyst [J ] . Applied Catalysis B: Environmental , 2023 , 324 : 122259 .
YANG J Y , PENG M , REN G Q , et al . A hydrothermally stable irreducible oxide-modified Pd/MgAl 2 O 4 catalyst for methane combustion [J ] . Angewandte Chemie International Edition , 2020 , 59 : 18522 - 18526 .
HUANG W X , JOHNSTON-PECK A C , WOLTER T , et al . Steam-created grain boundaries for methane C—H activation in palladium catalysts [J ] . Science , 2021 , 373 : 1518 - 1523 .
PENG H G , DONG T , YANG S Y , et al . Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes [J ] . Nature Communications , 2022 , 13 : 295 .
CARGNELLO M , JAÉN J J D , GARRIDO J C H , et al . Exceptional activity for methane combustion over modular Pd@CeO 2 subunits on functionalized Al 2 O 3 [J ] . Science , 2012 , 337 : 713 - 717 .
HOU Z Q , DAI L Y , DENG J G , et al . Electronically engineering water resistance in methane combustion with an atomically dispersed tungsten on PdO catalyst [J ] . Angewandte Chemie International Edition , 2022 , 61 : e202201655 .
FENG X L , GONG X R , LIU D P , et al . Bayesian optimization-guided discovery of high-performance methane combustion catalysts based on multi-component PtPd@CeZrO x core-shell nanospheres [J ] . Angewandte Chemie International Edition , 2023 , 62 : e202313068 .
JANG E J , LEE J , OH D G , et al . CH 4 oxidation act ivity in Pd and Pt-Pd bimetallic catalysts: Correlation with surface PdO x quantified from the DRIFTS study [J ] . ACS Catalysis , 2021 , 11 ( 10 ): 5894 - 5905 .
LOTT P , ECK M , DORONKIN D E , et al . Understanding sulfur poisoning of bimetallic Pd-Pt methane oxidation catalysts and their regeneration [J ] . Applied Catalysis B: Environmental , 2020 , 278 : 119244 .
XIONG H F , KUNWAR D , JIANG D , et al . Engineering catalyst supports to stabilize PdO x two-dimensional rafts for water-tolerant methane oxidation [J ] . Nature Catalysis , 2021 , 4 : 830 - 839 .
PARK J , KIM D , BYUN S W , et al . Impact of Pd:Pt ratio of Pd/Pt bimetallic catalyst on CH 4 oxidation [J ] . Applied catalysis B: Environmental , 2022 , 316 : 121623 .
PETROV A W , FERRI D , KRUMEICH F , et al . Stable complete methane oxidation over palladium based zeolite catalysts [J ] . Nature Communications , 2018 , 9 : 2545 .
WANG X B , ZHANG X Q , CAO M M , et al . Ordered mesoporous Pd-La/Al 2 O 3 catalysts for enhanced methane combustion [J ] . Energy & Fuels , 2022 , 36 ( 13 ): 6999 - 7005 .
HUANG X , EGGART D , QIN G Q , et al . Methyl radical chemistry in non-oxidative methane activation over metal single sites [J ] . Nature Communications , 2023 , 14 : 5716 .
EGGART D , HUANG X , ZIMINA A , et al . Operando XAS study of Pt-doped CeO 2 for the nonoxidative conversion of methane [J ] . ACS Catalysis , 2022 , 12 ( 7 ): 3897 - 3908 .
CARCAMO R A G , ZHANG X H , ESTEJAB A , et al . Differences of solvation thermodynamics of oxygenates at Pt/Al 2 O 3 perimeter versus Pt(111) terrace sites [J ] . iScience , 2023 , 26 ( 2 ), 105980 .
KWAK J H , HU J Z , MEI D H , et al . Coordinated unsaturated Al 3+ centers as binding sites for active catalyst phases of platinum on γ -Al 2 O 3 [J ] . Science , 2009 , 325 : 1670 - 1673 .
GUTIÉRREZ G , JOHANSSON B . Molecular dynamics study of structural properties of amorphous Al 2 O 3 [J ] . Physical Review B , 2002 , 65 : 104202 .
DESSAL C , SANGNIER A , CHIZALLET C , et al . Atmosphere-dependent stability and mobility of catalytic Pt single atoms and clusters on γ -Al 2 O 3 [J ] . Nanoscale , 2019 , 11 : 6897 - 6904 .
DUAN H M , YOU R , XU S T , et al . Pentacoordinated Al 3+ -stabilized active Pd structures on Al 2 O 3 -coated palladium catalysts for methane combustion [J ] . Angewandte Chemie International Edition , 2019 , 58 ( 35 ): 12043 - 12048 .
GOODMAN E D , DAI S , YANG A C , et al . Uniform Pt/Pd bimetallic nanocrystals demonstrate platinum effect on palladium methane combustion activity and stability [J ] . ACS Catalysis , 2017 , 7 ( 7 ): 4372 - 4380 .
NIE H Y , HOWE J Y , LACHKOV P T , et al . Chemical and structural dynamics of nanostructures in bimetallic Pt-Pd catalysts, their inhomogeneity, and their roles in methane oxidation [J ] . ACS Catalysis , 2019 , 9 ( 6 ): 5445 - 5460 .
NASSIRI H , LEE K E , HU Y F , et al . Water shifts PdO-catalyzed lean methane combustion to Pt-catalyzed rich combustion in Pd-Pt catalysts: In situ X-ray absorption spectroscopy [J ] . Journal of Catalysis , 2017 , 352 : 649 - 656 .
YIN F X , JI S F , WU P Y , et al . Deactivation behavior of Pd-based SBA-15 mesoporous silica catalysts for the catalytic combustion of methane [J ] . Journal of Catalysis , 2008 , 257 ( 1 ): 108 - 116 .
JANG G H , LEE E , JUNG H D , et al . Overcoming deactivation in wet methane combustion using Pd catalysts supported on mechanochemically mixed Al 2 O 3 and ZrO 2 [J ] . Chemical Engineering Journal , 2025 , 519 : 165468 .
LIU X Y , CHEN J K , HAN B W , et al . Lean methane combustion over zeolite-supported Pd catalysts: Structure-performance relationship and deactivation mechanism [J ] . Journal of Environmental Sciences , 2024 , 145 : 128 - 138 .
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