Precisely tuning the micro-nanoscale characteristics and synergistic effect of metal-acid sites to regulate the distribution of hydroconversion products are significant but challenging. The protonated carbocation intermediates triggered by tandem reaction on metal-acid region hinder target product formation due to their high reactivity and instability. Supported M/Zeolite hydroconversion catalysts, which often excel in simple synthesis, ease of separation and recyclability. However, they usually consist of sterically unconstrained metal centers which are isolated from acid sites, only providing limited coupling-selectivity to target product. Herein, metal nanoparticles enveloped in acidic zeolite frameworks were developed and used for investigating the process of hydroalkylation of benzene to cyclohexylbenzene. We show that appropriate metal encapsulation comprising adequate efficient metal-acid units successfully avoids the more thermodynamically favorable hydrogenation of cyclohexene to cyclohexane, but steers to alkylation of cyclohexene with benzene to cyclohexylbenzene. This resulted in the highest cyclohexylbenzene yield of 47.7% among the reported work, and surpassed the performance of all supported M/Zeolite catalysts. Experimental and theoretical results supported that the abundant bifunctional metal-acid units enhance the activation frequency and probability of intermediate cyclohexene. This work might provide insights for the integration strategy of dual active site and guidance for the construction of efficient “metal-acid balance” in tandem reactions.

Electrocatalytic reduction of CO₂ into high energy-density fuels and value-added chemicals under mild conditions can promote the sustainable cycle of carbon and decrease current energy and environmental problems. Constructing electrocatalyst with high activity, selectivity, stability, and low cost is really matter to realize industrial application of electrocatalytic CO₂ reduction (ECR). Metal–nitrogen–carbon (M–N–C), especially Ni–N–C, display excellent performance, such as nearly 100% CO selectivity, high current density, outstanding tolerance, etc., which is considered to possess broad application prospects. Based on the current research status, starting from the mechanism of ECR and the existence form of Ni active species, the latest research progress of Ni–N–C electrocatalysts in CO₂ electroreduction is systematically summarized. An overview is emphatically interpreted on the regulatory strategies for activity optimization over Ni–N–C, including N coordination modulation, vacancy defects construction, morphology design, surface modification, heteroatom activation, and bimetallic cooperation. Finally, some urgent problems and future prospects on designing Ni–N–C catalysts for ECR are discussed. This review aims to provide the guidance for the design and development of Ni–N–C catalysts with practical application.