利用Cu2+调控层状双氢氧化物电子结构促进CO2还原与塑料升级转化的选择性C2路径

doi:10.1016/S1872-2067(26)65182-0

催化学报 ›› 2026, Vol. 91: 103-121.DOI: 10.1016/S1872-2067(26)65182-0

利用Cu²⁺调控层状双氢氧化物电子结构促进CO₂还原与塑料升级转化的选择性C₂路径

罗健颖^a^,^b, 叶丰铭^a^,^b, 马宋哲^a^,^b, 曾宪海^c, 王伟俊^a^,^b^,^d^,^e^,^f^,^g^,^*()

^a 厦门大学马来西亚分校, 能源与化学工程学院, 雪兰莪州雪邦市, 马来西亚
^b 厦门大学纳米能源与催化技术卓越中心(CONNECT), 雪兰莪州雪邦市, 马来西亚
^c 厦门大学能源学院, 表界面化学全国重点实验室, 福建厦门 361102, 中国
^d 厦门大学化学化工学院, 表界面化学全国重点实验室, 福建厦门 361005, 中国
^e 厦门大学古雷石化研究院, 福建漳州 363200, 中国
^f 厦门大学深圳研究院, 广东深圳 518057, 中国
^g 高丽大学工程学院化学与生物工程系, 首尔, 韩国

收稿日期:2026-04-16 接受日期:2026-05-08 出版日期:2026-12-18 发布日期:2026-10-13
通讯作者: ^*电子信箱 : weejun.ong@xmu.edu.my (王伟俊).

Harnessing electronic structure modulation of Cu²⁺-mediated layered double hydroxide towards selective C₂ pathway in CO₂ reduction and plastic upcycling

Jian Yiing Loh^a^,^b, Feng Ming Yap^a^,^b, Elton Song-Zhe Mah^a^,^b, Xianhai Zeng^c, Wee-Jun Ong^a^,^b^,^d^,^e^,^f^,^g^,^*()

^a School of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^b Center of Excellence for NaNo Energy & Catalysis Technology (CONNECT), Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^c College of Energy, State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361102, Fujian, China
^d State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
^e Gulei Innovation Institute, Xiamen University, Zhangzhou 363200, Fujian, China
^f Shenzhen Research Institute of Xiamen University, Shenzhen 518057, Guangdong, China
^g Department of Chemical and Biological Engineering, College of Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul 02841, Republic of Korea

Received:2026-04-16 Accepted:2026-05-08 Online:2026-12-18 Published:2026-10-13

摘要/Abstract

摘要：

随着碳中和战略的推进以及塑料废弃物污染问题日益严峻, 开发兼具高效碳资源转化与废塑料升级利用功能的电催化体系需求日益增长, 本文旨在通过二氧化碳电化学还原与塑料升级转化相结合, 为高附加值C₂产物的绿色制备提供一条可持续途径. CO₂电还原反应(CO₂RR)能够将温室气体转化为高附加值燃料与化学品, 而聚对苯二甲酸乙二醇酯(PET)氧化反应(POR)则可实现废塑料资源化利用. 然而, 传统CO₂RR体系普遍存在C₂产物选择性低、反应动力学缓慢以及阳极析氧反应(OER)能耗较高等问题, 严重限制了实际应用. 因此, 构建兼具高效CO₂活化能力与PET氧化能力的双功能电催化剂, 对于实现低能耗、高附加值化学品协同制备具有重要意义. 基于此, 本文设计了一种CuMgAl层状双氢氧化物(LDH)与还原氧化石墨烯(rGO)耦合的自支撑异质结构催化剂, 通过调控Cu:Al比例实现电子结构优化, 以提升CO₂RR与POR过程中的C₂产物生成效率.
本研究成功构筑了CuMgAl层状双氢氧化物与还原氧化石墨烯复合材料(CMA-0.1-G), 作为兼具CO₂RR与POR功能的双功能电催化剂. 其分级化一维/三维纳米针结构可暴露大量催化活性位点, 同时加速电荷传输, 赋予催化剂长效稳定性能. 在CO₂RR性能方面, CMA-0.1-G在-1.0 V vs. RHE时实现了51.98%的C₂产物法拉第效率, 明显优于CMA-0.1 (24.09%)与MA (17.64%). 其Tafel斜率仅为32.35 mV dec^-1, 电荷转移电阻低至28.71 Ω, 说明其具有快速的电荷传输能力与优异的反应动力学性能. 这归因于Cu²⁺/Cu⁺/Cu⁰混合价态促进*CO吸附与C-C偶联. 原位拉曼光谱证实了*CO中间体的存在及其与Cu的强相互作用. 在PET升级氧化方面, CMA-0.1-G在1.58 V即可达到100 mA cm^-2电流密度, 明显优于其他对比样品, 并在50 mA cm^-2下稳定运行超过100 h, 草酸法拉第效率保持在89%以上, 得益于具有氧化还原活性的M-OOH物种的参与. 基于优异的双功能性能, 本文进一步构建了CMA-0.1-G||CMA-0.1-G双电极体系. 在耦合POR后, CO₂RR体系达到10 mA cm^-2仅需1.25 V, 远低于传统OER-CO₂RR, 体系的2.2 V. 流动池测试中, 该体系在3 V下连续稳定运行12 h, CO₂RR的平均C₂产物法拉第效率约45%, POR中草酸法拉第效率约55.85%. 进一步结合太阳能驱动后, 体系实现了5.68%的太阳能-燃料转换效率, 并在自然光条件下实现92%的草酸法拉第效率, 展现出良好的实际应用潜力.
综上, 本研究构建了一个多功能的CuMgAl-LDH/rGO异质结构, 实现了CO₂还原与PET升级氧化的高效耦合, 通过协同氧化还原反应实现C₂产物的高选择性生成, 为多碳产物定向生成与废塑料资源化利用提供了新策略. 该工作不仅揭示了Cu调控LDH电子结构及界面电场促进C-C偶联的机制, 同时也为开发低能耗、太阳能驱动的双功能电催化体系提供了理论基础与技术参考, 在绿色能源转化与可持续化学领域具有重要意义.

关键词: 二氧化碳还原反应, 层状双氢氧化物, 双功能, 聚对苯二甲酸乙二酯, C₂产物

Abstract:

The integration of CO₂ electroreduction with plastic upcycling offers a sustainable route to generate high-value C₂ products. This study presents a self-supported CuMgAl layered double hydroxide coupled with reduced graphene oxide (CMA-0.1-G) as a bifunctional electrocatalyst for both CO₂ reduction (CO₂RR) and polyethylene terephthalate (PET) oxidation (POR). The hierarchical 1D/3D nanoneedle structure enables abundant active sites, efficient charge transport, and high stability. CMA-0.1-G achieves a 51.98% Faradaic efficiency (FE) for C₂ products during CO₂RR, attributed to mixed Cu²⁺/Cu⁺/Cu⁰ oxidation states that promote *CO adsorption and C-C coupling. In-situ Raman spectroscopy confirms *CO intermediates and strong Cu-CO interactions. For POR, the catalyst demonstrates an impressive > 89% FE toward C₂ oxidation products, aided by redox-active M-OOH species. A two-electrode bifunctional system using CMA-0.1-G for both CO₂RR and POR is assembled and operates at 1.25 V for 10 mA cm^-2. In addition, the catalysts were tested using flow cell, demonstrating impressive performance for over 12 h under high voltage. Density functional theory analysis reveals the key intermediates formation, adsorption and desorption of the intermediates on key catalytic active sites, offering mechanistic insights into the optimum catalyst. Under simulated sunlight, the system achieves 5.68% solar-to-fuel efficiency for CO₂RR and 92% FE for oxalic acid. This work establishes a multifunctional, scalable platform for coupling CO₂RR and plastic upcycling, selectively generating C₂ products through coordinated redox reactions, offering a viable solution for carbon neutrality and circular chemical manufacturing.

Key words: CO₂ reduction reaction, Layered double hydroxide, Bifunctional, Polyethylene terephthalate, C₂ products

罗健颖, 叶丰铭, 马宋哲, 曾宪海, 王伟俊. 利用Cu²⁺调控层状双氢氧化物电子结构促进CO₂还原与塑料升级转化的选择性C₂路径[J]. 催化学报, 2026, 91: 103-121.

Jian Yiing Loh, Feng Ming Yap, Elton Song-Zhe Mah, Xianhai Zeng, Wee-Jun Ong. Harnessing electronic structure modulation of Cu²⁺-mediated layered double hydroxide towards selective C₂ pathway in CO₂ reduction and plastic upcycling[J]. Chinese Journal of Catalysis, 2026, 91: 103-121.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65182-0

https://www.cjcatal.com/CN/Y2026/V91/I12/103

图/表 8

Fig. 1. (a) Schematic illustration of the synthesis of CMA-0.1-G. FESEM images of CMA-0.1-G on copper foam with elevating magnifications of 10 μm (b), 1 μm (c,d), and 200 nm (e). (f) STEM image with the corresponding EDX mapping of Cu, Mg, Al, C and O elements of CMA-0.1-G. (g) EDX spectrum of Cu, Mg, Al, C and O in CMA-0.1-G.

Fig. 2. (a) Low magnification TEM image of CMA-0.1-G, with the inset highlighting the CuMgAl-LDH. (b) HRTEM image of CMA-0.1-G with inset of FFT image. (c) Magnified TEM image of CMA-0.1-G. (d) HRTEM image of nanoneedles LDH. (e) XRD patterns of CMA-0.1 and CMA-0.1-G. (f) Raman spectra of CMA-0.1 and CMA-0.1-G.

Fig. 3. XPS spectra of C 1s (a), O 1s (b), Cu 2p (c), Cu LMM (d), Mg 1s (e), Mg 2p (f) and Al 2p (g). BET analysis (h) and pore size distribution (i) of CMA-0.1-G and CMA-0.1.

Fig. 4. Electrocatalytic CO2RR Performance. (a) LSV plots for different catalysts. Tafel plots (b), Nyquist plots (c), and Cdl (d) for the as-prepared catalysts. (e) FE values of C1 and C2 products at various applied potentials for CMA-0.1-G. (f) C2 partial current density plot of MA, CMA-0.1 and CMA-0.1-G. (g) Comparison plot of typical CO2RR electrocatalysts (e.g. MgAl-LDH/Cu [6], Ni/Cu [48], CuZn@Al-fum [49], CeO2-Cu2O/GA [50], Cu-N4/C [51], Ag-Cu2OPB [52], Cu-complex/Cu [10] and Cu@Ag-2 NPs [53]). (h) Chronopotentiometry test of CMA-0.1-G at 50 mA cm-2 for 100 h.

Fig. 5. (a) Graphical illustration of C2 product formation from electrocatalyst. In-situ Raman spectra for CO2RR for CMA-0.1 in the range of 400-780 cm-1 (b), 800-1100 cm-1 (c), 1900-2180 cm-1 (d) and CMA-0.1-G in the range of 400-800 cm-1 (e), 900-1150 cm-1 (f), and 1300-2200 cm-1 (g) at a potential range of -0.7 to -1.3 V vs. RHE. (h) Free energy profiles of CO2RR on MA and CMA-0.1 catalysts.

Fig. 6. Electrocatalytic PET oxidation performance. LSV plot (a), Tafel plot (b), Nyquist plot (c) and electrochemical double layer capacitance (Cdl) (d) for the as-prepared catalysts. (e) Chronopotentiometry test and FE of CMA-0.1-G at 50 mA cm-2 for 100 h.

Fig. 7. In-situ Raman spectra for CMA-0.1-G during OER (1 mol L-1 KOH) in the range of 350-750 cm-1 (a), 900-1300 cm-1 (b), 1400-1900 cm-1 (c) and PET oxidation at potential range of -0.7 to -1.3 V vs. RHE (d). (e) OER (1 mol L-1 KOH) and half-way injected PET under 1.7 V. (f) PET oxidation reaction network and free energy diagram for PET oxidation to oxalic acid on the surfaces of CMA-0.1 and MA.

Fig. 8. (a) LSV polarization curves of the integrated cell with and without PET hydrolysate. Flow-cell bifunctional electrolyzer: chronoamperometry stability test for POR-CO2RR. Chronoamperometry for CO2RR with product FE (b) and chronoamperometry for POR with product FE (c). CO2RR (d) and POR (e) stability during continuous illumination for 12 h, along with the inset displaying the solar-cell (light on and light off) bifunctional POR-CO2RR hybrid unit featuring CMA-0.1-G as the anode and cathode electrodes. (f) The ηSTF of the tested electrocatalysts in bifunctional solar-powered electrolysis at the 60th min.

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利用Cu²⁺调控层状双氢氧化物电子结构促进CO₂还原与塑料升级转化的选择性C₂路径

Harnessing electronic structure modulation of Cu²⁺-mediated layered double hydroxide towards selective C₂ pathway in CO₂ reduction and plastic upcycling

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