CuWOx纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇

doi:10.1016/S1872-2067(25)64898-4

催化学报 ›› 2026, Vol. 84: 347-358.DOI: 10.1016/S1872-2067(25)64898-4

CuWO_x纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇

邹洁琪^a, 何迁^b, 刘雷^a(), 赵斌彬^c(), 董晋湘^a()

^a 太原理工大学化学与化工学院, 化学产品工程山西省重点实验室, 山西太原030024, 中国
^b 新加坡国立大学材料科学与工程系, 新加坡
^c 太原科技大学化学工程与技术学院, 山西太原030024, 中国

收稿日期:2025-09-16 接受日期:2025-10-02 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: liulei@tyut.edu.cn (刘雷),
binbinzhao1121@163.com (赵斌彬),
dongjinxiangwork@hotmail.com (董晋湘).
基金资助:
国家自然科学基金(22478276);国家自然科学基金(22408253);国家自然科学基金(21978194);山西省科技创新团队专项经费(202204051001009)

Precise construction of Pt-O-W active sites via atom replacement on CuWO_x nanoislands for efficient glycerol hydrogenolysis to 1,3-propanediol

Jieqi Zou^a, Qian He^b, Lei Liu^a(), Binbin Zhao^c(), Jinxiang Dong^a()

^a Shanxi Key Laboratory of Chemical Product Engineering, College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^b Department of Materials Science and Engineering, National University of Singapore, Singapore
^c School of Chemical Engineering and Technology, Taiyuan University of Science and Technology, Taiyuan 030024, Shanxi, China

Received:2025-09-16 Accepted:2025-10-02 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: liulei@tyut.edu.cn (L. Liu),
binbinzhao1121@163.com (B. Zhao),
dongjinxiangwork@hotmail.com (J. Dong).
Supported by:
National Natural Science Foundation(22478276);National Natural Science Foundation(22408253);National Natural Science Foundation(21978194);Special Fund for Science and Technology Innovation Teams of Shanxi Province(202204051001009)

摘要/Abstract

摘要：

界面效应在多相催化反应中具有重要作用. 尽管界面工程已被广泛研究, 但对负载型双功能催化剂而言, 在载体表面构建结构均一、明确的双金属界面仍面临巨大挑战. Pt-WO_x体系因具备金属加氢与酸催化功能, 被视为工业级甘油氢解最具前途的催化体系之一. 然而, 如何同时提高甘油氢解转化效率与1,3-PDO选择性仍是重大挑战. 尽管目前已认识到Pt-WO_x界面位点在促进C-O键断裂中的关键作用, 但实现对WO_x纳米结构及Pt在金属-氧化物界面空间分布的精确调控仍具有挑战性. 因此, 本文旨在开发一种先进的Pt-WO_x界面工程控制策略, 通过在Pt与WO_x之间构建精准的空间构型和电子相互作用, 实现CO₂加氢制甲醇反应路径的精确调控并提升催化稳定性.

本研究提出一种Pt-WO_x纳米原子层覆盖策略, 在紧凑空间内精准调控金属-载体相互作用, 构建具有更高原子利用效率的双功能界面. 该策略以Cu为空间介导和锚定位点, 诱导Pt选择性沉积于CuWO_x纳米岛上, 形成结构明确、高密度的单一Pt-WO_x活性中心, 从而制备出富含Pt-WO_x界面活性位点的Pt-WO_x/γ-Al₂O₃复合催化剂. 该催化剂在高甘油浓度(30.0 wt%)下实现65%的1,3-丙二醇(1,3-PDO)选择性和0.302 g_1,3-PDO·g_cat^-1·h^-1的时空产率. 通过球差校正透射电子显微镜证实了CuWO_x的形态特征: 均匀分散的纳米岛平均尺寸为0.59 nm, PtO_x在这些岛上实现了精准定位. 利用原位物质吸附-红外光谱实验系统阐明了甘油在Pt-WO_x界面吸/脱附的动态过程, Cu修饰的Pt-WO_x活性位点促进了甘油分子的吸附. 此外, X射线光电子能谱、原位H₂漫反射傅立叶变换红外光谱及H₂程序升温脱附实验结果显示, Cu物种可调控Pt-WO_x中心的电子态, 证明Pt-Cu置换策略不仅能保持Pt物种高分散、抑制团聚, 还利用Cu⁰作为电子助剂强化了Pt-WO_x相互作用; 同时, Pt与Cu间的协同作用促进氢溢流跨越Pt-WO_x界面, 极大提升了H₂吸附/解离能力, 使总吸氢量提升至1.23 mmol·g^-1, 为传统催化剂Pt/WO_x/γ-Al₂O₃的两倍, 这种精准构筑的Pt-WO_x活性位点为甘油氢解提供了更为充足的活性氢. 基于实验证据、表征数据与机理认识, 对不同Pt基催化剂上甘油氢解制1,3-PDO提出了两条截然不同的反应路径. 在Pt-WO_x/γ-Al₂O₃体系中, 催化中心位于Pt-WO_x纳米岛. 甘油分子的伯羟基吸附于岛面; H₂在Pt位点异裂解离, 生成H^δ⁺与H^δ^-. H^δ^-锚定于PtO_x, 而H^δ⁺溢流至WO_x岛, 原位形成位于Pt-WO_x界面的W-OH布朗斯特酸位. W-OH布朗斯特酸位与甘油仲羟基作用, 生成表面束缚的仲碳正离子, 随即被邻近的Pt-H^δ^-快速攻击, 最终脱附得到1,3-PDO. Pt-H^δ^-与W-OH在空间上紧密相邻、协同作用, 是高1,3-PDO选择性的根源. 相反, Pt/WO_x/γ-Al₂O₃的Pt-WO_x界面密度低, 质子溢流受限, Pt-(OH)-W活性中心难以动态形成, W-OH生成受阻, Pt-H^δ^-与W-OH的协同效应被削弱, 导致1,3-PDO选择性显著下降.

综上, 本研究提出的“Pt-WO_x纳米岛”策略, 在氧化铝载体表面成功构筑了均一、明确的双金属界面, 为纳米岛合成提供了新思路, 也为负载型金属-氧化物催化剂的界面精准设计提供了新见解, 并有望拓展至其它反应体系.

关键词: 多相催化, 铂-钨催化剂, 甘油加氢脱氧反应, 纳米岛, 1,3-丙二醇

Abstract:

Interfacial engineering is central to heterogeneous catalytic hydrogenation. However, achieving the precise control of bimetallic interfaces in supported bifunctional catalysts remains a critical issue. Herein, we present a strategic atom-replacement approach in which Cu acts as a spatial mediator and anchoring site, enabling Pt to be selectively deposited onto CuWO_x nanoislands, thereby forming well-defined high-density Pt-WO_x active sites for the selective hydrogenolysis of glycerol. The characterization results demonstrate that Cu species modulate the electronic states of the Pt-WO_x centers, while the cooperative interaction between Pt and Cu enhances the hydrogen spillover across the Pt-WO_x interface. This synergy promotes the formation of 1,3-propanediol (1,3-PDO) by optimizing the reaction pathway. Consequently, the Pt-WO_x/γ-Al₂O₃ catalyst achieved 65% selectivity to 1,3-PDO with a space-time yield of 0.302 g_1,3-PDO·g_cat^-1·h^-1 at a high glycerol concentration (30.0 wt%), outperforming all previously reported Al₂O₃-based systems. This work not only provides a new approach for nanoisland synthesis, but also offers valuable insights into interfacial control in heterogeneous catalysis.

Key words: Heterogeneous catalysis, Pt-W catalyst, Glycerol hydrodeoxygenation, Nanoisland, 1,3-Propanediol

邹洁琪, 何迁, 刘雷, 赵斌彬, 董晋湘. CuWO_x纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇[J]. 催化学报, 2026, 84: 347-358.

Jieqi Zou, Qian He, Lei Liu, Binbin Zhao, Jinxiang Dong. Precise construction of Pt-O-W active sites via atom replacement on CuWO_x nanoislands for efficient glycerol hydrogenolysis to 1,3-propanediol[J]. Chinese Journal of Catalysis, 2026, 84: 347-358.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64898-4

https://www.cjcatal.com/CN/Y2026/V84/I5/347

图/表 8

Scheme 1. Procedure for the synthesis of homogeneous and highly dispersed “nanoisland” cluster catalysts.

Fig. 1. Structural characterization and electron microscopy images of nanoislands. (a) XRD patterns of different catalysts. (b) FT-IR patterns to determine the structure of CuWOx. (c) UV-vis patterns of the catalysts before and after the addition of Cu. AC-high-angle angular dark-field (HAADF)-STEM and EDS mapping images of CuWOx/γ-Al2O3 (d-f) and Pt-WOx/γ-Al2O3 (g-i). (e1,h1) are the HAADF intensity maps obtained by point-by-point scanning of atoms along the line marked in (e2,h2).

Table 1 Basic parameters of the sample.

Samples	C_Pt^a (wt%)	C_W^a (wt%)	C_Cu^a (wt%)	Cu/W atomic ratio^a	D_Pt^b (%)	H₂^c (mmol·g^-1)	NH₃^d (mmol·g^-1)
CuWO_x/γ-Al₂O₃	—	5.42	0.84	0.45	—	0.24	0.70
WO_x/γ-Al₂O₃	—	5.33	—	—	—	0.17	0.59
Pt-WO_x/γ-Al₂O₃	1.87	5.34	0.16	0.09	61.36	1.23	1.41
Pt/WO_x/γ-Al₂O₃	1.98	5.25	—	—	58.94	0.56	1.07

Fig. 2. In-situ FT-IR and XPS investigations of the electron transfer between Pt and W and the strength of Cu-mediated interactions. (a) In-situ DRIFTS spectra of CO chemisorption on the CuWOx/γ-Al2O3 sample. (b) Corresponding Gaussian fitting of CO-DRIFTS spectra for the Pt-WOx/γ-Al2O3 sample. XPS spectra of Pt-WOx/γ-Al2O3 and Pt/WOx/γ-Al2O3 in the Pt 4f (c), W 4f (d), and O 1s (e) regions. (f) In-situ DRIFTS spectra of CO chemisorption on Pt-WOx/γ-Al2O3 and Pt/WOx/γ-Al2O3 samples.

Fig. 3. Catalyst performance tests. (a) Catalytic performance of various catalysts in the glycerol hydrogenation reaction (150 °C). (b) Impact of different reaction temperatures on the catalytic performance (12 h). (c) Comparison of the 1,3-PDO productivity and Pt efficiency among current aluminum-containing Pt-W catalytic systems for glycerol hydrodeoxygenation. Detailed data are also compiled in Table S4.

Fig. 4. Analysis of the ability of the catalyst to dissociate and activate H2. In-situ H2-DRIFTS of CuWOx/γ-Al2O3 (a) and two Pt-containing catalysts (b,c), together with an enlarged comparison (d). H2-TPD profiles (e) and comparative H2 uptake (f) of the different catalysts.

Fig. 5. Adsorption and hydrogenolysis of glycerol. (a) Adsorption configuration of glycerol on Pt-WOx nanoislands. Liquid FT-IR spectra of glycerol, 1,3-PDO, 1,2-PDO (b) compared with the FT-IR spectra of glycerol (c) adsorbed on γ-Al2O3. (d) FT-IR spectra of glycerol adsorption on CuWOx/γ-Al2O3 with temperature adsorption and desorption. In-situ FT-IR spectra of glycerol on Pt-WOx/γ-Al2O3 (e) and Pt/WOx/γ-Al2O3 (f) under Ar-H2 atmosphere switching. (g) Desorption plots of the intensity ratio of primary to secondary hydroxyl groups with increasing temperature on γ-Al2O3 and CuWOx/γ-Al2O3. (h) Comparison of magnified plots of the changes in the intensity of primary and secondary hydroxyl groups after switching H2 in Fig. (e). (i) H2-TPR spectra of different sample surfaces.

Fig. 6. Catalyst surface acidity and mechanism. NH3-TPD spectra of different catalysts (a) and results of Gaussian peak fitting in the highly acidic region of Pt-containing samples (b). (c) Pyridine adsorption FT-IR spectra of Pt-containing samples collected at 150 °C. Real-time H2 adsorption IR spectra of NH3 adsorption on Pt-WOx/γ-Al2O3 (d), Pt/WOx/γ-Al2O3 (e), and CuWOx/γ-Al2O3 (f) after Ar blowdown and 1 h of NH3 adsorption collected at 100 °C. Glycerol adsorption hydrogenolysis mechanism diagram over Pt-containing catalysts prepared by atom replacement (g) and impregnation (h) methods.

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CuWO_x纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇

Precise construction of Pt-O-W active sites via atom replacement on CuWO_x nanoislands for efficient glycerol hydrogenolysis to 1,3-propanediol

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CuWOx纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇

Precise construction of Pt-O-W active sites via atom replacement on CuWOx nanoislands for efficient glycerol hydrogenolysis to 1,3-propanediol

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CuWO_x纳米岛原子置换精准构筑Pt-O-W活性位高效催化甘油氢解制1,3-丙二醇

Precise construction of Pt-O-W active sites via atom replacement on CuWO_x nanoislands for efficient glycerol hydrogenolysis to 1,3-propanediol